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Title: Substitutional Growth of Methylammonium Lead Iodide Perovskites in Alcohols

Methylammonium lead iodide (MAPbI 3) perovskites are organic–inorganic semiconductors with long carrier diffusion lengths serving as the light-harvesting component in optoelectronics. Through a substitutional growth of MAPbI 3 catalyzed by polar protic alcohols, evidence is shown in this paper for their substrate- and annealing-free production and use of toxic solvents and high temperature is prevented. The resulting variable-sized crystals (≈100 nm–10 µm) are found to be tetragonally single-phased in alcohols and precipitated as powders that are metallic-lead-free. A comparatively low MAPbI 3 yield in toluene supports the role of alcohol polarity and the type of solvent (protic vs aprotic). The theoretical calculations suggest that overall Gibbs free energy in alcohols is lowered due to their catalytic impact. Based on this alcohol-catalyzed approach, MAPbI 3 is obtained, which is chemically stable in air up to ≈1.5 months and thermally stable (≤300 °C). Finally, this method is amendable to large-scale manufacturing and ultimately can lead to energy-efficient, low-cost, and stable devices.
Authors:
 [1] ;  [2] ;  [3] ;  [3] ;  [3] ;  [3] ;  [4] ;  [5] ;  [5] ;  [1] ;  [6]
  1. Argonne National Lab. (ANL), Argonne, IL (United States). Center for Nanoscale Materials. Nanoscience and Technology Division
  2. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States). Dept. of Organic Materials Science
  3. Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source. X-Ray Science Division
  4. Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division
  5. Ulsan National Inst. of Science and Technology (UNIST), Ulsan (Korea, Republic of). Dept. of Chemistry
  6. (United States). Inst. for Molecular Engineering
Publication Date:
Grant/Contract Number:
AC02-06CH11357; NA0003525
Type:
Accepted Manuscript
Journal Name:
Advanced Energy Materials
Additional Journal Information:
Journal Volume: 8; Journal Issue: 5; Journal ID: ISSN 1614-6832
Publisher:
Wiley
Research Org:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE National Nuclear Security Administration (NNSA)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Alcohols; Crystal Growth; Perovskites; Solar Cells; Stability
OSTI Identifier:
1427505
Alternate Identifier(s):
OSTI ID: 1395602

Acik, Muge, Alam, Todd M., Guo, Fangmin, Ren, Yang, Lee, Byeongdu, Rosenberg, Richard A., Mitchell, John F., Park, In Kee, Lee, Geunsik, Darling, Seth B., and Univ. of Chicago, IL. Substitutional Growth of Methylammonium Lead Iodide Perovskites in Alcohols. United States: N. p., Web. doi:10.1002/aenm.201701726.
Acik, Muge, Alam, Todd M., Guo, Fangmin, Ren, Yang, Lee, Byeongdu, Rosenberg, Richard A., Mitchell, John F., Park, In Kee, Lee, Geunsik, Darling, Seth B., & Univ. of Chicago, IL. Substitutional Growth of Methylammonium Lead Iodide Perovskites in Alcohols. United States. doi:10.1002/aenm.201701726.
Acik, Muge, Alam, Todd M., Guo, Fangmin, Ren, Yang, Lee, Byeongdu, Rosenberg, Richard A., Mitchell, John F., Park, In Kee, Lee, Geunsik, Darling, Seth B., and Univ. of Chicago, IL. 2017. "Substitutional Growth of Methylammonium Lead Iodide Perovskites in Alcohols". United States. doi:10.1002/aenm.201701726. https://www.osti.gov/servlets/purl/1427505.
@article{osti_1427505,
title = {Substitutional Growth of Methylammonium Lead Iodide Perovskites in Alcohols},
author = {Acik, Muge and Alam, Todd M. and Guo, Fangmin and Ren, Yang and Lee, Byeongdu and Rosenberg, Richard A. and Mitchell, John F. and Park, In Kee and Lee, Geunsik and Darling, Seth B. and Univ. of Chicago, IL},
abstractNote = {Methylammonium lead iodide (MAPbI3) perovskites are organic–inorganic semiconductors with long carrier diffusion lengths serving as the light-harvesting component in optoelectronics. Through a substitutional growth of MAPbI3 catalyzed by polar protic alcohols, evidence is shown in this paper for their substrate- and annealing-free production and use of toxic solvents and high temperature is prevented. The resulting variable-sized crystals (≈100 nm–10 µm) are found to be tetragonally single-phased in alcohols and precipitated as powders that are metallic-lead-free. A comparatively low MAPbI3 yield in toluene supports the role of alcohol polarity and the type of solvent (protic vs aprotic). The theoretical calculations suggest that overall Gibbs free energy in alcohols is lowered due to their catalytic impact. Based on this alcohol-catalyzed approach, MAPbI3 is obtained, which is chemically stable in air up to ≈1.5 months and thermally stable (≤300 °C). Finally, this method is amendable to large-scale manufacturing and ultimately can lead to energy-efficient, low-cost, and stable devices.},
doi = {10.1002/aenm.201701726},
journal = {Advanced Energy Materials},
number = 5,
volume = 8,
place = {United States},
year = {2017},
month = {9}
}

Works referenced in this record:

Organometal Halide Perovskites as Visible-Light Sensitizers for Photovoltaic Cells
journal, May 2009
  • Kojima, Akihiro; Teshima, Kenjiro; Shirai, Yasuo
  • Journal of the American Chemical Society, Vol. 131, Issue 17, p. 6050-6051
  • DOI: 10.1021/ja809598r

High-quality bulk hybrid perovskite single crystals within minutes by inverse temperature crystallization
journal, July 2015
  • Saidaminov, Makhsud I.; Abdelhady, Ahmed L.; Murali, Banavoth
  • Nature Communications, Vol. 6, Article No. 7586
  • DOI: 10.1038/ncomms8586

Solvent engineering for high-performance inorganic–organic hybrid perovskite solar cells
journal, July 2014
  • Jeon, Nam Joong; Noh, Jun Hong; Kim, Young Chan
  • Nature Materials, Vol. 13, Issue 9, p. 897-903
  • DOI: 10.1038/nmat4014

Density‐functional thermochemistry. III. The role of exact exchange
journal, April 1993
  • Becke, Axel D.
  • The Journal of Chemical Physics, Vol. 98, Issue 7, p. 5648-5652
  • DOI: 10.1063/1.464913

Sequential deposition as a route to high-performance perovskite-sensitized solar cells
journal, July 2013
  • Burschka, Julian; Pellet, Norman; Moon, Soo-Jin
  • Nature, Vol. 499, Issue 7458, p. 316-319
  • DOI: 10.1038/nature12340

Synthesis and Characterization of Organic−Inorganic Perovskite Thin Films Prepared Using a Versatile Two-Step Dipping Technique
journal, January 1998
  • Liang, Kangning; Mitzi, David B.; Prikas, Michael T.
  • Chemistry of Materials, Vol. 10, Issue 1, p. 403-411
  • DOI: 10.1021/cm970568f

Electron-Hole Diffusion Lengths Exceeding 1 Micrometer in an Organometal Trihalide Perovskite Absorber
journal, October 2013
  • Stranks, S. D.; Eperon, G. E.; Grancini, G.
  • Science, Vol. 342, Issue 6156, p. 341-344
  • DOI: 10.1126/science.1243982

A facile solvothermal growth of single crystal mixed halide perovskite CH3NH3Pb(Br1−xClx)3
journal, January 2015
  • Zhang, Taiyang; Yang, Mengjin; Benson, Eric E.
  • Chemical Communications, Vol. 51, Issue 37, p. 7820-7823
  • DOI: 10.1039/C5CC01835H