Substitutional Growth of Methylammonium Lead Iodide Perovskites in Alcohols

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.

doi:10.1002/aenm.201701726

Title: Substitutional Growth of Methylammonium Lead Iodide Perovskites in Alcohols

Journal Article · Fri Sep 29 00:00:00 EDT 2017 · Advanced Energy Materials

DOI:https://doi.org/10.1002/aenm.201701726· OSTI ID:1427505

Acik, Muge ^[1]; Alam, Todd M. ^[2]; Guo, Fangmin ^[3]; Ren, Yang ^[3]; Lee, Byeongdu ^[3]; Rosenberg, Richard A. ^[3]; Mitchell, John F. ^[4]; Park, In Kee ^[5]; Lee, Geunsik ^[5]; Darling, Seth B. ^[1]

Argonne National Lab. (ANL), Argonne, IL (United States). Center for Nanoscale Materials. Nanoscience and Technology Division
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States). Dept. of Organic Materials Science
Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source. X-Ray Science Division
Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division
Ulsan National Inst. of Science and Technology (UNIST), Ulsan (Korea, Republic of). Dept. of Chemistry

Abstract 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 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). This method is amendable to large‐scale manufacturing and ultimately can lead to energy‐efficient, low‐cost, and stable devices.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC02-06CH11357; NA0003525; DE‐AC02‐06CH11357; DE‐NA0003525

OSTI ID:: 1427505

Alternate ID(s):: OSTI ID: 1395602

Journal Information:: Advanced Energy Materials, Vol. 8, Issue 5; ISSN 1614-6832

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 22 works

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References (58)

Dipolar Aprotic Solvents in Bimolecular Aromatic Nucleophilic Substitution Reactions ¹ Miller, J.; Parker, Alan J. Journal of the American Chemical Society, Vol. 83, Issue 1 https://doi.org/10.1021/ja01462a023	journal	January 1961
The role of databases in support of computational chemistry calculations Feller, David Journal of Computational Chemistry, Vol. 17, Issue 13 https://doi.org/10.1002/(SICI)1096-987X(199610)17:13<1571::AID-JCC9>3.0.CO;2-P	journal	October 1996
Bulk crystal growth of hybrid perovskite material CH ₃ NH ₃ PbI ₃ Dang, Yangyang; Liu, Yang; Sun, Youxuan CrystEngComm, Vol. 17, Issue 3 https://doi.org/10.1039/C4CE02106A	journal	January 2015
Low trap-state density and long carrier diffusion in organolead trihalide perovskite single crystals Shi, D.; Adinolfi, V.; Comin, R. Science, Vol. 347, Issue 6221 https://doi.org/10.1126/science.aaa2725	journal	January 2015
Metal halide perovskites for energy applications Zhang, Wei; Eperon, Giles E.; Snaith, Henry J. Nature Energy, Vol. 1, Issue 6 https://doi.org/10.1038/nenergy.2016.48	journal	May 2016
Hydration of methylamine and methylammonium ion: structural and thermodynamic properties from the data of the integral equation method in the RISM approximation Fedotova, M. V.; Kruchinin, S. E. Russian Chemical Bulletin, Vol. 61, Issue 2 https://doi.org/10.1007/s11172-012-0034-5	journal	February 2012
Improved performance and stability of perovskite solar cells by crystal crosslinking with alkylphosphonic acid ω-ammonium chlorides Li, Xiong; Ibrahim Dar, M.; Yi, Chenyi Nature Chemistry, Vol. 7, Issue 9 https://doi.org/10.1038/nchem.2324	journal	August 2015
Organometal Halide Perovskites as Visible-Light Sensitizers for Photovoltaic Cells Kojima, Akihiro; Teshima, Kenjiro; Shirai, Yasuo Journal of the American Chemical Society, Vol. 131, Issue 17, p. 6050-6051 https://doi.org/10.1021/ja809598r	journal	May 2009
Investigation of moisture stability and PL characteristics of terpineol-passivated organic–inorganic hybrid perovskite Guo, Xin; McCleese, Christopher; Gao, Weiyin Materials for Renewable and Sustainable Energy, Vol. 5, Issue 4 https://doi.org/10.1007/s40243-016-0081-1	journal	September 2016
Unreacted PbI ₂ as a Double-Edged Sword for Enhancing the Performance of Perovskite Solar Cells Jacobsson, T. Jesper; Correa-Baena, Juan-Pablo; Halvani Anaraki, Elham Journal of the American Chemical Society, Vol. 138, Issue 32 https://doi.org/10.1021/jacs.6b06320	journal	August 2016
GSAS-II : the genesis of a modern open-source all purpose crystallography software package Toby, Brian H.; Von Dreele, Robert B. Journal of Applied Crystallography, Vol. 46, Issue 2 https://doi.org/10.1107/S0021889813003531	journal	March 2013
Reproducible Fabrication of Efficient Perovskite-based Solar Cells: X-ray Crystallographic Studies on the Formation of CH ₃ NH ₃ PbI ₃ Layers Wakamiya, Atsushi; Endo, Masaru; Sasamori, Takahiro Chemistry Letters, Vol. 43, Issue 5 https://doi.org/10.1246/cl.140074	journal	May 2014
Chemical and Electronic Structure Characterization of Lead Halide Perovskites and Stability Behavior under Different Exposures—A Photoelectron Spectroscopy Investigation Philippe, Bertrand; Park, Byung-Wook; Lindblad, Rebecka Chemistry of Materials, Vol. 27, Issue 5 https://doi.org/10.1021/acs.chemmater.5b00348	journal	February 2015
A combined single crystal neutron/X-ray diffraction and solid-state nuclear magnetic resonance study of the hybrid perovskites CH ₃ NH ₃ PbX ₃ (X = I, Br and Cl) Baikie, Tom; Barrow, Nathan S.; Fang, Yanan Journal of Materials Chemistry A, Vol. 3, Issue 17 https://doi.org/10.1039/C5TA01125F	journal	January 2015
Hysteresis-less inverted CH ₃ NH ₃ PbI ₃ planar perovskite hybrid solar cells with 18.1% power conversion efficiency Heo, Jin Hyuck; Han, Hye Ji; Kim, Dasom Energy & Environmental Science, Vol. 8, Issue 5 https://doi.org/10.1039/C5EE00120J	journal	January 2015
Relationships between Lead Halide Perovskite Thin-Film Fabrication, Morphology, and Performance in Solar Cells Sharenko, Alexander; Toney, Michael F. Journal of the American Chemical Society, Vol. 138, Issue 2 https://doi.org/10.1021/jacs.5b10723	journal	November 2015
High-quality bulk hybrid perovskite single crystals within minutes by inverse temperature crystallization Saidaminov, Makhsud I.; Abdelhady, Ahmed L.; Murali, Banavoth Nature Communications, Vol. 6, Article No. 7586 https://doi.org/10.1038/ncomms8586	journal	July 2015
Visualizing Carrier Diffusion in Individual Single-Crystal Organolead Halide Perovskite Nanowires and Nanoplates Tian, Wenming; Zhao, Chunyi; Leng, Jing Journal of the American Chemical Society, Vol. 137, Issue 39 https://doi.org/10.1021/jacs.5b08045	journal	September 2015
Solvent engineering for high-performance inorganic–organic hybrid perovskite solar cells Jeon, Nam Joong; Noh, Jun Hong; Kim, Young Chan Nature Materials, Vol. 13, Issue 9, p. 897-903 https://doi.org/10.1038/nmat4014	journal	July 2014
Dielectric Constants of Water, Methanol, Ethanol, Butanol and Acetone: Measurement and Computational Study Mohsen-Nia, M.; Amiri, H.; Jazi, B. Journal of Solution Chemistry, Vol. 39, Issue 5 https://doi.org/10.1007/s10953-010-9538-5	journal	May 2010
Organometal halide perovskite solar cells: degradation and stability Berhe, Taame Abraha; Su, Wei-Nien; Chen, Ching-Hsiang Energy & Environmental Science, Vol. 9, Issue 2 https://doi.org/10.1039/C5EE02733K	journal	January 2016
Thermal Behavior of Methylammonium Lead-Trihalide Perovskite Photovoltaic Light Harvesters Dualeh, Amalie; Gao, Peng; Seok, Sang Il Chemistry of Materials, Vol. 26, Issue 21 https://doi.org/10.1021/cm502468k	journal	October 2014
Atomistic Origins of High-Performance in Hybrid Halide Perovskite Solar Cells Frost, Jarvist M.; Butler, Keith T.; Brivio, Federico Nano Letters, Vol. 14, Issue 5 https://doi.org/10.1021/nl500390f	journal	April 2014
Selective dissolution of halide perovskites as a step towards recycling solar cells Kim, Byeong Jo; Kim, Dong Hoe; Kwon, Seung Lee Nature Communications, Vol. 7, Issue 1 https://doi.org/10.1038/ncomms11735	journal	May 2016
Direct Crystallization Route to Methylammonium Lead Iodide Perovskite from an Ionic Liquid Moore, David T.; Tan, Kwan W.; Sai, Hiroaki Chemistry of Materials, Vol. 27, Issue 9 https://doi.org/10.1021/cm5047484	journal	April 2015
Pathways toward high-performance perovskite solar cells: review of recent advances in organo-metal halide perovskites for photovoltaic applications Song, Zhaoning; Watthage, Suneth C.; Phillips, Adam B. Journal of Photonics for Energy, Vol. 6, Issue 2 https://doi.org/10.1117/1.JPE.6.022001	journal	April 2016
Tracking the formation of methylammonium lead triiodide perovskite Liu, Lijia; McLeod, John A.; Wang, Rongbin Applied Physics Letters, Vol. 107, Issue 6 https://doi.org/10.1063/1.4928662	journal	August 2015
Mayer Bond Order as a Metric of Complexation Effectiveness in Lead Halide Perovskite Solutions Stevenson, James; Sorenson, Blaire; Subramaniam, Varun Hari Chemistry of Materials, Vol. 29, Issue 6 https://doi.org/10.1021/acs.chemmater.6b04327	journal	November 2016
Ultrasmooth organic–inorganic perovskite thin-film formation and crystallization for efficient planar heterojunction solar cells Zhang, Wei; Saliba, Michael; Moore, David T. Nature Communications, Vol. 6, Issue 1 https://doi.org/10.1038/ncomms7142	journal	January 2015
Hydrogen bond network relaxation resolved by alcohol hydration (methanol, ethanol, and glycerol): Alcohol-induced hydrogen-bond network relaxation Gong, Yinyan; Xu, Yan; Zhou, Yong Journal of Raman Spectroscopy, Vol. 48, Issue 3 https://doi.org/10.1002/jrs.5060	journal	November 2016
Impact of Processing Temperature and Composition on the Formation of Methylammonium Lead Iodide Perovskites Song, Zhaoning; Watthage, Suneth C.; Phillips, Adam B. Chemistry of Materials, Vol. 27, Issue 13 https://doi.org/10.1021/acs.chemmater.5b01017	journal	June 2015
Density‐functional thermochemistry. III. The role of exact exchange Becke, Axel D. The Journal of Chemical Physics, Vol. 98, Issue 7, p. 5648-5652 https://doi.org/10.1063/1.464913	journal	April 1993
Solution-Grown Monocrystalline Hybrid Perovskite Films for Hole-Transporter-Free Solar Cells Peng, Wei; Wang, Lingfei; Murali, Banavoth Advanced Materials, Vol. 28, Issue 17 https://doi.org/10.1002/adma.201506292	journal	March 2016
Toward Tailored Film Morphologies: The Origin of Crystal Orientation in Hybrid Perovskite Thin Films Oesinghaus, Lukas; Schlipf, Johannes; Giesbrecht, Nadja Advanced Materials Interfaces, Vol. 3, Issue 19 https://doi.org/10.1002/admi.201600403	journal	October 2016
Enhanced optoelectronic quality of perovskite thin films with hypophosphorous acid for planar heterojunction solar cells Zhang, Wei; Pathak, Sandeep; Sakai, Nobuya Nature Communications, Vol. 6, Issue 1 https://doi.org/10.1038/ncomms10030	journal	November 2015
Development of the Colle-Salvetti correlation-energy formula into a functional of the electron density Lee, Chengteh; Yang, Weitao; Parr, Robert G. Physical Review B, Vol. 37, Issue 2 https://doi.org/10.1103/PhysRevB.37.785	journal	January 1988
Sequential deposition as a route to high-performance perovskite-sensitized solar cells Burschka, Julian; Pellet, Norman; Moon, Soo-Jin Nature, Vol. 499, Issue 7458, p. 316-319 https://doi.org/10.1038/nature12340	journal	July 2013
Stripping down SN2 Orr-Ewing, Andrew J. Nature Chemistry, Vol. 4, Issue 7 https://doi.org/10.1038/nchem.1377	journal	June 2012
Mechanism for rapid growth of organic–inorganic halide perovskite crystals Nayak, Pabitra K.; Moore, David T.; Wenger, Bernard Nature Communications, Vol. 7, Issue 1 https://doi.org/10.1038/ncomms13303	journal	November 2016
On the Thermal and Thermodynamic (In)Stability of Methylammonium Lead Halide Perovskites Brunetti, Bruno; Cavallo, Carmen; Ciccioli, Andrea Scientific Reports, Vol. 6, Issue 1 https://doi.org/10.1038/srep31896	journal	August 2016
CH ₃ NH ₃ PbCl ₃ Single Crystals: Inverse Temperature Crystallization and Visible-Blind UV-Photodetector Maculan, Giacomo; Sheikh, Arif D.; Abdelhady, Ahmed L. The Journal of Physical Chemistry Letters, Vol. 6, Issue 19 https://doi.org/10.1021/acs.jpclett.5b01666	journal	September 2015
Synthesis and Characterization of Organic−Inorganic Perovskite Thin Films Prepared Using a Versatile Two-Step Dipping Technique Liang, Kangning; Mitzi, David B.; Prikas, Michael T. Chemistry of Materials, Vol. 10, Issue 1, p. 403-411 https://doi.org/10.1021/cm970568f	journal	January 1998
Solution Growth of Single Crystal Methylammonium Lead Halide Perovskite Nanostructures for Optoelectronic and Photovoltaic Applications Fu, Yongping; Meng, Fei; Rowley, Matthew B. Journal of the American Chemical Society, Vol. 137, Issue 17 https://doi.org/10.1021/jacs.5b02651	journal	April 2015
Electron-Hole Diffusion Lengths Exceeding 1 Micrometer in an Organometal Trihalide Perovskite Absorber Stranks, S. D.; Eperon, G. E.; Grancini, G. Science, Vol. 342, Issue 6156, p. 341-344 https://doi.org/10.1126/science.1243982	journal	October 2013
Making and Breaking of Lead Halide Perovskites Manser, Joseph S.; Saidaminov, Makhsud I.; Christians, Jeffrey A. Accounts of Chemical Research, Vol. 49, Issue 2 https://doi.org/10.1021/acs.accounts.5b00455	journal	January 2016
Crystal Growth and Dissolution of Methylammonium Lead Iodide Perovskite in Sequential Deposition: Correlation between Morphology Evolution and Photovoltaic Performance Hsieh, Tsung-Yu; Huang, Chi-Kai; Su, Tzu-Sen ACS Applied Materials & Interfaces, Vol. 9, Issue 10 https://doi.org/10.1021/acsami.6b12303	journal	March 2017
Enhanced Photoluminescence and Solar Cell Performance via Lewis Base Passivation of Organic–Inorganic Lead Halide Perovskites Noel, Nakita K.; Abate, Antonio; Stranks, Samuel D. ACS Nano, Vol. 8, Issue 10 https://doi.org/10.1021/nn5036476	journal	September 2014
Gas-phase hydration reactions of protonated alcohols. Energetics and bulk hydration of cluster ions Hiraoka, K.; Takimoto, H.; Morise, K. Journal of the American Chemical Society, Vol. 108, Issue 19 https://doi.org/10.1021/ja00279a004	journal	September 1986
Low surface recombination velocity in solution-grown CH3NH3PbBr3 perovskite single crystal Yang, Ye; Yan, Yong; Yang, Mengjin Nature Communications, Vol. 6, Issue 1 https://doi.org/10.1038/ncomms8961	journal	August 2015
One-step, low-temperature deposited perovskite solar cell utilizing small molecule additive Chen, Chun-Chao; Hong, Zirou; Li, Gang Journal of Photonics for Energy, Vol. 5, Issue 1 https://doi.org/10.1117/1.JPE.5.057405	journal	January 2015
Towards stable and commercially available perovskite solar cells Park, Nam-Gyu; Grätzel, Michael; Miyasaka, Tsutomu Nature Energy, Vol. 1, Issue 11 https://doi.org/10.1038/nenergy.2016.152	journal	October 2016
A facile solvothermal growth of single crystal mixed halide perovskite CH₃NH₃Pb(Br_1−xCl_x)₃ Zhang, Taiyang; Yang, Mengjin; Benson, Eric E. Chemical Communications, Vol. 51, Issue 37, p. 7820-7823 https://doi.org/10.1039/C5CC01835H	journal	January 2015
Stability of Organic Cations in Solution-Processed CH ₃ NH ₃ PbI ₃ Perovskites: Formation of Modified Surface Layers Calloni, A.; Abate, A.; Bussetti, G. The Journal of Physical Chemistry C, Vol. 119, Issue 37 https://doi.org/10.1021/acs.jpcc.5b05422	journal	September 2015
Methylammonium lead triiodide perovskite solar cells: A new paradigm in photovoltaics Nazeeruddin, Mohammad Khaja; Snaith, Henry MRS Bulletin, Vol. 40, Issue 8 https://doi.org/10.1557/mrs.2015.169	journal	August 2015
Formation of Thin Films of Organic-Inorganic Perovskites for High-Efficiency Solar Cells Stranks, Samuel D.; Nayak, Pabitra K.; Zhang, Wei Angewandte Chemie International Edition, Vol. 54, Issue 11 https://doi.org/10.1002/anie.201410214	journal	February 2015
Persistent Dopants and Phase Segregation in Organolead Mixed-Halide Perovskites Rosales, Bryan A.; Men, Long; Cady, Sarah D. Chemistry of Materials, Vol. 28, Issue 19 https://doi.org/10.1021/acs.chemmater.6b01874	journal	August 2016
The solubility of some sparingly soluble lead salts: An evaluation of the solubility in water and aqueous electrolyte solution Clever, H. Lawrence; Johnston, Francis J. Journal of Physical and Chemical Reference Data, Vol. 9, Issue 3 https://doi.org/10.1063/1.555628	journal	July 1980
The effects of solvation on the properties of anions in dipolar aprotic solvents Parker, A. J. Quarterly Reviews, Chemical Society, Vol. 16, Issue 2 https://doi.org/10.1039/qr9621600163	journal	January 1962

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