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Lead Chalcogenide Nanoparticles and Their Size-Controlled Self-Assemblies for Thermoelectric and Photovoltaic Applications

  • Caleb K. Miskin
    Caleb K. Miskin
    Davidson School of Chemical Engineering, Purdue University, West Lafayette, Indiana 47907, United States
  • Swapnil D. Deshmukh
    Swapnil D. Deshmukh
    Davidson School of Chemical Engineering, Purdue University, West Lafayette, Indiana 47907, United States
  • Venkata Vasiraju
    Venkata Vasiraju
    Department of Chemical Engineering, Texas A&M University, College Station, Texas 77843, United States
  • Kevin Bock
    Kevin Bock
    Davidson School of Chemical Engineering, Purdue University, West Lafayette, Indiana 47907, United States
    More by Kevin Bock
  • Gaurav Mittal
    Gaurav Mittal
    Davidson School of Chemical Engineering, Purdue University, West Lafayette, Indiana 47907, United States
  • Angela Dubois-Camacho
    Angela Dubois-Camacho
    Davidson School of Chemical Engineering, Purdue University, West Lafayette, Indiana 47907, United States
  • Sreeram Vaddiraju
    Sreeram Vaddiraju
    Department of Chemical Engineering, Texas A&M University, College Station, Texas 77843, United States
  • , and 
  • Rakesh Agrawal*
    Rakesh Agrawal
    Davidson School of Chemical Engineering, Purdue University, West Lafayette, Indiana 47907, United States
    *E-mail: [email protected]
Cite this: ACS Appl. Nano Mater. 2019, 2, 3, 1242–1252
Publication Date (Web):February 1, 2019
https://doi.org/10.1021/acsanm.8b02125
Copyright © 2019 American Chemical Society

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    Abstract

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    We report a facile, room temperature synthesis of PbS, PbSe, PbSxSe1–x, and PbTe nanoparticles and their microscale assemblies by combining a chalcogen solution and a lead halide solution in select thiol–amine mixtures. Selection of an appropriate thiol–amine pair and/or the use of appropriate amine to thiol ratio has demonstrated a size control on nanoparticle self-assemblies ranging from nano- to microscale. Proper washing of these particles has yielded phase-pure and compositionally uniform material with minimal or no presence of any carbonaceous ligands on the particle surface, making it attractive for electronic device fabrication. The resulting PbS material exhibits bandgaps in the range 0.6 eV to as high as 1.2 eV for various assembly sizes. These optical bandgaps confirm the retention of quantum confinement of PbS material even in self-assembled nano/microstructures, which could be an interesting phenomenon for future photovoltaic development. Along with carbon-free, quantum-confined self-assemblies, this chemistry also provides a room temperature and instantaneous reaction route to synthesize individually dispersed PbS and PbSe particles with long chain ligand capping similar to traditional synthesis routes. The PbSe material synthesized from this route shows the ability to alloy with PbS at room temperature in the entire composition range and also demonstrates thermoelectric performance comparable to results in existing undoped PbSe literature.

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acsanm.8b02125.

    • Observations on material compatibility for thiol–amine mixtures, additional SEM and TEM images for lead chalcogenide nanoparticles synthesized at various conditions, tabulated data on solubility limit of PbS in various thiol–amine pairs, 1H NMR data on PbS microsphere, STEM-EDS data on PbS0.75Se0.25 alloy particle (PDF)

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    Cited By

    This article is cited by 19 publications.

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