DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Highly Porous Thermoelectric Nanocomposites with Low Thermal Conductivity and High Figure of Merit from Large-Scale Solution-Synthesized Bi2Te2.5Se0.5 Hollow Nanostructures

Abstract

To enhance the performance of thermoelectric materials and enable access to their widespread applications, it is beneficial yet challenging to synthesize hollow nanostructures in large quantities, with high porosity, low thermal conductivity (κ) and excellent figure of merit ($$z$$T). Herein we report a scalable (ca. 11.0 g per batch) and low-temperature colloidal processing route for Bi2Te2.5Se0.5 hollow nanostructures. They are sintered into porous, bulk nanocomposites (phi 10 mm×h 10 mm) with low κ (0.48 W m-1 K-1) and the highest z T (1.18) among state-of-the-art Bi2Te3-xSex materilas. Additional benefits of the unprecedented low relative density (68–77 %) are the large demand reduction of raw materials and the improved portability. This method can be adopted to fabricate other porous phase-transition and thermoelectric chalcogenide materials and will pave the way for the implementation of hollow nanostructures in other fields.

Authors:
 [1];  [2];  [3];  [4];  [2];  [3];  [1]
  1. Iowa State Univ., Ames, IA (United States). Dept. of Chemical and Biological Engineering; Ames Lab., Ames, IA (United States)
  2. Purdue Univ., West Lafayette, IN (United States). Dept. of Mechanical Engineering
  3. Northwestern Univ., Evanston, IL (United States). Dept. of Materials Science and Engineering
  4. Ames Lab., Ames, IA (United States)
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Solid-State Solar-Thermal Energy Conversion Center (S3TEC)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); US Department of the Navy, Office of Naval Research (ONR); Defense Advanced Research Projects Agency (DARPA)
OSTI Identifier:
1470457
Alternate Identifier(s):
OSTI ID: 1401264
Grant/Contract Number:  
SC0001299; FG02-09ER46577; AC02-07CH11358
Resource Type:
Accepted Manuscript
Journal Name:
Angewandte Chemie (International Edition)
Additional Journal Information:
Journal Name: Angewandte Chemie (International Edition); Journal Volume: 56; Journal Issue: 13; Related Information: S3TEC partners with Massachusetts Institute of Technology (lead); Boston College; Oak Ridge National Laboratory; Rensselaer Polytechnic Institute; Journal ID: ISSN 1433-7851
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 42 ENGINEERING; 77 NANOSCIENCE AND NANOTECHNOLOGY; hollow nanostructures; Kirkendall effect; porous nanocomposites; thermal conductivity; thermoelectric materials; solar (photovoltaic); solar (thermal); solid state lighting; phonons; thermoelectric; defects; mechanical behavior; charge transport; spin dynamics; materials and chemistry by design; optics; synthesis (novel materials); synthesis (self-assembly); synthesis (scalable processing)

Citation Formats

Xu, Biao, Feng, Tianli, Agne, Matthias T., Zhou, Lin, Ruan, Xiulin, Snyder, G. Jeffery, and Wu, Yue. Highly Porous Thermoelectric Nanocomposites with Low Thermal Conductivity and High Figure of Merit from Large-Scale Solution-Synthesized Bi2Te2.5Se0.5 Hollow Nanostructures. United States: N. p., 2017. Web. doi:10.1002/anie.201612041.
Xu, Biao, Feng, Tianli, Agne, Matthias T., Zhou, Lin, Ruan, Xiulin, Snyder, G. Jeffery, & Wu, Yue. Highly Porous Thermoelectric Nanocomposites with Low Thermal Conductivity and High Figure of Merit from Large-Scale Solution-Synthesized Bi2Te2.5Se0.5 Hollow Nanostructures. United States. https://doi.org/10.1002/anie.201612041
Xu, Biao, Feng, Tianli, Agne, Matthias T., Zhou, Lin, Ruan, Xiulin, Snyder, G. Jeffery, and Wu, Yue. Thu . "Highly Porous Thermoelectric Nanocomposites with Low Thermal Conductivity and High Figure of Merit from Large-Scale Solution-Synthesized Bi2Te2.5Se0.5 Hollow Nanostructures". United States. https://doi.org/10.1002/anie.201612041. https://www.osti.gov/servlets/purl/1470457.
@article{osti_1470457,
title = {Highly Porous Thermoelectric Nanocomposites with Low Thermal Conductivity and High Figure of Merit from Large-Scale Solution-Synthesized Bi2Te2.5Se0.5 Hollow Nanostructures},
author = {Xu, Biao and Feng, Tianli and Agne, Matthias T. and Zhou, Lin and Ruan, Xiulin and Snyder, G. Jeffery and Wu, Yue},
abstractNote = {To enhance the performance of thermoelectric materials and enable access to their widespread applications, it is beneficial yet challenging to synthesize hollow nanostructures in large quantities, with high porosity, low thermal conductivity (κ) and excellent figure of merit ($z$T). Herein we report a scalable (ca. 11.0 g per batch) and low-temperature colloidal processing route for Bi2Te2.5Se0.5 hollow nanostructures. They are sintered into porous, bulk nanocomposites (phi 10 mm×h 10 mm) with low κ (0.48 W m-1 K-1) and the highest z T (1.18) among state-of-the-art Bi2Te3-xSex materilas. Additional benefits of the unprecedented low relative density (68–77 %) are the large demand reduction of raw materials and the improved portability. This method can be adopted to fabricate other porous phase-transition and thermoelectric chalcogenide materials and will pave the way for the implementation of hollow nanostructures in other fields.},
doi = {10.1002/anie.201612041},
journal = {Angewandte Chemie (International Edition)},
number = 13,
volume = 56,
place = {United States},
year = {Thu Jan 12 00:00:00 EST 2017},
month = {Thu Jan 12 00:00:00 EST 2017}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 123 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Monocrystalline spinel nanotube fabrication based on the Kirkendall effect
journal, July 2006

  • Jin fan, Hong; Knez, Mato; Scholz, Roland
  • Nature Materials, Vol. 5, Issue 8
  • DOI: 10.1038/nmat1673

Interface Engineering in Solution-Processed Nanocrystal Thin Films for Improved Thermoelectric Performance
journal, October 2016


Thinking Like a Chemist: Intuition in Thermoelectric Materials
journal, April 2016

  • Zeier, Wolfgang G.; Zevalkink, Alex; Gibbs, Zachary M.
  • Angewandte Chemie International Edition, Vol. 55, Issue 24
  • DOI: 10.1002/anie.201508381

A Mesoporous Anisotropic n-Type Bi 2 Te 3 Monolith with Low Thermal Conductivity as an Efficient Thermoelectric Material
journal, July 2012

  • Zhang, Yichi; Day, Tristan; Snedaker, Matthew L.
  • Advanced Materials, Vol. 24, Issue 37
  • DOI: 10.1002/adma.201201974

A Thermoelectric Zintl Phase Na 2+ x Ga 2+ x Sn 4- x with Disordered Na Atoms in Helical Tunnels
journal, July 2015

  • Yamada, Takahiro; Yamane, Hisanori; Nagai, Hideaki
  • Advanced Materials, Vol. 27, Issue 32
  • DOI: 10.1002/adma.201501970

New and Old Concepts in Thermoelectric Materials
journal, November 2009

  • Sootsman, Joseph R.; Chung, Duck Young; Kanatzidis, Mercouri G.
  • Angewandte Chemie International Edition, Vol. 48, Issue 46, p. 8616-8639
  • DOI: 10.1002/anie.200900598

Effects of nanoscale porosity on thermoelectric properties of SiGe
journal, May 2010

  • Lee, Hohyun; Vashaee, Daryoosh; Wang, D. Z.
  • Journal of Applied Physics, Vol. 107, Issue 9
  • DOI: 10.1063/1.3388076

Cubic AgPbmSbTe2+m: Bulk Thermoelectric Materials with High Figure of Merit
journal, February 2004


New Directions for Low-Dimensional Thermoelectric Materials
journal, April 2007

  • Dresselhaus, M. S.; Chen, G.; Tang, M. Y.
  • Advanced Materials, Vol. 19, Issue 8, p. 1043-1053
  • DOI: 10.1002/adma.200600527

Formation of Hollow Nanocrystals Through the Nanoscale Kirkendall Effect
journal, April 2004


Synthesis, Properties, and Applications of Hollow Micro-/Nanostructures
journal, May 2016


Modular Inorganic Nanocomposites by Conversion of Nanocrystal Superlattices
journal, March 2010

  • Tangirala, Ravisubhash; Baker, Jessy L.; Alivisatos, A. Paul
  • Angewandte Chemie, Vol. 122, Issue 16
  • DOI: 10.1002/ange.200906642

Large-scale solution-phase production of Bi2Te3 and PbTe nanowires using Te nanowire templates
journal, January 2014

  • Finefrock, Scott W.; Fang, Haiyu; Yang, Haoran
  • Nanoscale, Vol. 6, Issue 14
  • DOI: 10.1039/c4nr01191k

Tuning Multiscale Microstructures to Enhance Thermoelectric Performance of n-Type Bismuth-Telluride-Based Solid Solutions
journal, June 2015


PbS/PbSe Hollow Spheres: Solvothermal Synthesis, Growth Mechanism, and Thermoelectric Transport Property
journal, July 2012

  • Jin, Rencheng; Chen, Gang; Pei, Jian
  • The Journal of Physical Chemistry C, Vol. 116, Issue 30
  • DOI: 10.1021/jp302206q

Facile synthesis of ultrahigh-surface-area hollow carbon nanospheres for enhanced adsorption and energy storage
journal, June 2015

  • Xu, Fei; Tang, Zhiwei; Huang, Siqi
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms8221

Vibrations in binary and ternary topological insulators: First-principles calculations and Raman spectroscopy measurements
journal, November 2012


Experimental Studies on Anisotropic Thermoelectric Properties and Structures of n-Type Bi2Te2.7Se0.3
journal, September 2010

  • Yan, Xiao; Poudel, Bed; Ma, Yi
  • Nano Letters, Vol. 10, Issue 9, p. 3373-3378
  • DOI: 10.1021/nl101156v

Convergence of Conduction Bands as a Means of Enhancing Thermoelectric Performance of n -Type Mg 2 Si 1 x Sn x Solid Solutions
journal, April 2012


Modular Inorganic Nanocomposites by Conversion of Nanocrystal Superlattices
journal, March 2010

  • Tangirala, Ravisubhash; Baker, Jessy L.; Alivisatos, A. Paul
  • Angewandte Chemie International Edition, Vol. 49, Issue 16, p. 2878-2882
  • DOI: 10.1002/anie.200906642

Template-Free Synthesis of SnO2 Hollow Nanostructures with High Lithium Storage Capacity
journal, September 2006

  • Lou, X. W.; Wang, Y.; Yuan, C.
  • Advanced Materials, Vol. 18, Issue 17, p. 2325-2329
  • DOI: 10.1002/adma.200600733

Control of the nanoscale crystallinity in mesoporous TiO 2 shells for enhanced photocatalytic activity
journal, January 2012

  • Joo, Ji Bong; Zhang, Qiao; Dahl, Michael
  • Energy Environ. Sci., Vol. 5, Issue 4
  • DOI: 10.1039/C1EE02533C

Fabrication of Hollow Palladium Spheres and Their Successful Application to the Recyclable Heterogeneous Catalyst for Suzuki Coupling Reactions
journal, July 2002

  • Kim, Sang-Wook; Kim, Minsuk; Lee, Wha Young
  • Journal of the American Chemical Society, Vol. 124, Issue 26, p. 7642-7643
  • DOI: 10.1021/ja026032z

Facile synthesis of Ag nanocubes and Au nanocages
journal, September 2007


Studies on the Bi 2 Te 3 –Bi 2 Se 3 –Bi 2 S 3 system for mid-temperature thermoelectric energy conversion
journal, January 2013

  • Liu, Weishu; Lukas, Kevin C.; McEnaney, Kenneth
  • Energy Environ. Sci., Vol. 6, Issue 2
  • DOI: 10.1039/C2EE23549H

Alte und neue Konzepte für thermoelektrische Materialien
journal, November 2009

  • Sootsman, Joseph R.; Chung, Duck Young; Kanatzidis, Mercouri G.
  • Angewandte Chemie, Vol. 121, Issue 46
  • DOI: 10.1002/ange.200900598

Denken wie ein Chemiker: Thermoelektrika intuitiv
journal, April 2016

  • Zeier, Wolfgang G.; Zevalkink, Alex; Gibbs, Zachary M.
  • Angewandte Chemie, Vol. 128, Issue 24
  • DOI: 10.1002/ange.201508381

A general analytical approach toward the thermal conductivity of porous media
journal, November 1993


High-Thermoelectric Performance of Nanostructured Bismuth Antimony Telluride Bulk Alloys
journal, May 2008


Bioinspired hollow semiconductor nanospheres as photosynthetic nanoparticles
journal, January 2012

  • Sun, Jianhua; Zhang, Jinshui; Zhang, Mingwen
  • Nature Communications, Vol. 3, Issue 1
  • DOI: 10.1038/ncomms2152

Colloidal Synthesis of Hollow Cobalt Sulfide Nanocrystals
journal, July 2006

  • Yin, Y.; Erdonmez, C. K.; Cabot, A.
  • Advanced Functional Materials, Vol. 16, Issue 11
  • DOI: 10.1002/adfm.200600256

Enhanced Thermoelectric Properties of Solution Grown Bi2Te3–xSex Nanoplatelet Composites
journal, February 2012

  • Soni, Ajay; Yanyuan, Zhao; Ligen, Yu
  • Nano Letters, Vol. 12, Issue 3, p. 1203-1209
  • DOI: 10.1021/nl2034859

New Directions for Low-Dimensional Thermoelectric Materials
journal, June 2007

  • Dresselhaus, Mildred S.; Chen, Gang; Tang, Ming Y.
  • ChemInform, Vol. 38, Issue 26
  • DOI: 10.1002/chin.200726202

Works referencing / citing this record:

Synergistic Compositional-Mechanical-Thermal Effects Leading to a Record High zT in n-Type V 2 VI 3 Alloys Through Progressive Hot Deformation
journal, July 2018

  • Hu, Lipeng; Zhang, Yang; Wu, Haijun
  • Advanced Functional Materials, Vol. 28, Issue 35
  • DOI: 10.1002/adfm.201803617

Large-Scale, Solution-Synthesized Nanostructured Composites for Thermoelectric Applications
journal, August 2018


Self‐Templating Approaches to Hollow Nanostructures
journal, July 2018


Progress of Photodetectors Based on the Photothermoelectric Effect
journal, July 2019


Are Cu 2 Te‐Based Compounds Excellent Thermoelectric Materials?
journal, October 2019


Thermoelectric materials: The power of pores
journal, February 2017


High thermoelectric performance of n-type Bi 2 Te 2.7 Se 0.3 via nanostructure engineering
journal, January 2018

  • Li, D.; Li, J. M.; Li, J. C.
  • Journal of Materials Chemistry A, Vol. 6, Issue 20
  • DOI: 10.1039/c8ta00525g

Dual defect system of tellurium antisites and silver interstitials in off-stoichiometric Bi 2 (Te,Se) 3+y causing enhanced thermoelectric performance
journal, January 2019

  • Kim, Cham; Lopez, David Humberto; Kim, Dong Hwan
  • Journal of Materials Chemistry A, Vol. 7, Issue 2
  • DOI: 10.1039/c8ta05261a

Compositionally tunable ternary Bi 2 (Se 1−x Te x ) 3 and (Bi 1−y Sb y ) 2 Te 3 thin films via low pressure chemical vapour deposition
journal, January 2018

  • Benjamin, Sophie L.; de Groot, C. H. (Kees); Gurnani, Chitra
  • Journal of Materials Chemistry C, Vol. 6, Issue 29
  • DOI: 10.1039/c8tc01285g

Interfacial energy band and phonon scattering effect in Bi 2 Te 3 -polypyrrole hybrid thermoelectric material
journal, October 2018

  • Kim, Cham; Baek, Ju Young; Lopez, David Humberto
  • Applied Physics Letters, Vol. 113, Issue 15
  • DOI: 10.1063/1.5050089

Thermoelectric properties improvement in quasi-one-dimensional organic crystals
journal, November 2019

  • Sanduleac, Ionel; Pflaum, Jens; Casian, Anatolie
  • Journal of Applied Physics, Vol. 126, Issue 17
  • DOI: 10.1063/1.5120461

High‐Performance Solution‐Processable Flexible SnSe Nanosheet Films for Lower Grade Waste Heat Recovery
journal, February 2019


Advances in thermoelectrics
journal, April 2018