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Title: Solvent-free synthesis of organometallic halides CH3NH3PbI3 and (CH3NH3)3Bi2I9 and their thermoelectric transport properties

Abstract

Organometallic halides are great candidates for optoelectronics. As an important family of semiconductors, understanding their thermoelectric transport properties is also important. This has been a challenging task as many of such compounds are highly intrinsic. In this work, we synthesized two halides, CH3NH3PbI3 and (CH3NH3)3Bi2I9, using a solvent-free method. We found an extraordinarily high Seebeck coefficient of +2600 ± 200 μV/K in (CH3NH3)3Bi2I9. For CH3NH3PbI3, our synthesis method led to a negative Seebeck coefficient of –1350 ± 50 μV/K, in contrast to positive values observed in solvent synthesized samples. We also found the thermal conductivity of CH3NH3PbI3 to be 0.38 W/m K, largely independent of temperature from 300 K to 450 K, despite a tetragonal-to-cubic phase transition. (CH3NH3)3Bi2I9 has an even lower thermal conductivity of 0.21 W/m K (also temperature independent) which is due to its soft phonon dispersion and weak bonds.

Authors:
 [1];  [1];  [2]; ORCiD logo [2]; ORCiD logo [1]
  1. Illinois Inst. of Technology, Chicago, IL (United States)
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). The Molecular Foundry
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1567169
Alternate Identifier(s):
OSTI ID: 1557028
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Applied Physics Letters
Additional Journal Information:
Journal Volume: 115; Journal Issue: 7; Journal ID: ISSN 0003-6951
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Long, Xiang, Pan, Zhenyu, Zhang, Zhuolei, Urban, Jeffrey J., and Wang, Heng. Solvent-free synthesis of organometallic halides CH3NH3PbI3 and (CH3NH3)3Bi2I9 and their thermoelectric transport properties. United States: N. p., 2019. Web. doi:10.1063/1.5113535.
Long, Xiang, Pan, Zhenyu, Zhang, Zhuolei, Urban, Jeffrey J., & Wang, Heng. Solvent-free synthesis of organometallic halides CH3NH3PbI3 and (CH3NH3)3Bi2I9 and their thermoelectric transport properties. United States. https://doi.org/10.1063/1.5113535
Long, Xiang, Pan, Zhenyu, Zhang, Zhuolei, Urban, Jeffrey J., and Wang, Heng. 2019. "Solvent-free synthesis of organometallic halides CH3NH3PbI3 and (CH3NH3)3Bi2I9 and their thermoelectric transport properties". United States. https://doi.org/10.1063/1.5113535. https://www.osti.gov/servlets/purl/1567169.
@article{osti_1567169,
title = {Solvent-free synthesis of organometallic halides CH3NH3PbI3 and (CH3NH3)3Bi2I9 and their thermoelectric transport properties},
author = {Long, Xiang and Pan, Zhenyu and Zhang, Zhuolei and Urban, Jeffrey J. and Wang, Heng},
abstractNote = {Organometallic halides are great candidates for optoelectronics. As an important family of semiconductors, understanding their thermoelectric transport properties is also important. This has been a challenging task as many of such compounds are highly intrinsic. In this work, we synthesized two halides, CH3NH3PbI3 and (CH3NH3)3Bi2I9, using a solvent-free method. We found an extraordinarily high Seebeck coefficient of +2600 ± 200 μV/K in (CH3NH3)3Bi2I9. For CH3NH3PbI3, our synthesis method led to a negative Seebeck coefficient of –1350 ± 50 μV/K, in contrast to positive values observed in solvent synthesized samples. We also found the thermal conductivity of CH3NH3PbI3 to be 0.38 W/m K, largely independent of temperature from 300 K to 450 K, despite a tetragonal-to-cubic phase transition. (CH3NH3)3Bi2I9 has an even lower thermal conductivity of 0.21 W/m K (also temperature independent) which is due to its soft phonon dispersion and weak bonds.},
doi = {10.1063/1.5113535},
url = {https://www.osti.gov/biblio/1567169}, journal = {Applied Physics Letters},
issn = {0003-6951},
number = 7,
volume = 115,
place = {United States},
year = {Tue Aug 13 00:00:00 EDT 2019},
month = {Tue Aug 13 00:00:00 EDT 2019}
}

Journal Article:
Free Publicly Available Full Text
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Citation Metrics:
Cited by: 14 works
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Figures / Tables:

FIG. 1 FIG. 1: (a) XRD pattern of CH3NH3PbI3 powder after different times of mechanical alloying; reference pattern from PDF 01-085-5509. (b) XRD pattern of (CH3NH3)3Bi2I9 after 30 min of mechanical alloying; reference pattern from PDF 01-085-6014. (c) Absorption spectrum of the two halides at room temperature. (d) TGA weight loss ofmore » the two halides.« less

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Works referencing / citing this record:

Tackling Challenges in Seebeck Coefficient Measurement of Ultra‐High Resistance Samples with an AC Technique
journal, January 2020


Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.