Skip to main content
U.S. Department of Energy
Office of Scientific and Technical Information

Substitutional Growth of Methylammonium Lead Iodide Perovskites in Alcohols

Journal Article · · Advanced Energy Materials
 [1];  [2];  [3];  [3];  [3];  [3];  [4];  [5];  [5];  [6]
  1. Center for Nanoscale Materials, Nanoscience and Technology Division, Argonne National Laboratory, Lemont IL 60439 USA
  2. Department of Organic Materials Science, Sandia National Laboratory, Albuquerque NM 87185 USA
  3. Advanced Photon Source, X-Ray Science Division, Argonne National Laboratory, Lemont IL 60439 USA
  4. Materials Science Division, Argonne National Laboratory, Lemont IL 60439 USA
  5. Department of Chemistry, Ulsan National Institute of Science and Technology (UNIST), Ulsan 44919 South Korea
  6. Center for Nanoscale Materials, Nanoscience and Technology Division, Argonne National Laboratory, Lemont IL 60439 USA; Institute for Molecular Engineering, University of Chicago, 5640 South Ellis Avenue Chicago IL 60637 USA
Methylammonium lead iodide (MAPbIx) perovskites are organic-inorganic semiconductors that serve as the light-harvesting component in photovoltaic devices. Their long carrier diffusion lengths yield power conversion efficiencies in excess of 22%. Conventional growth techniques apply spin-coated precursors on an oxide or polymer substrate followed by annealing; however, use of toxic solvents and high temperature hinder device stability and performance. Through a nucleophilic substitutional growth of MAPbIx in polar protic alcohols, we show evidence for their substrate- and annealing- free production. These 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 with a negligibly small amount of unreacted PbI2 (<10%). On the basis of this chemical approach, we obtain chemically stable MAPbIx in air up to ~1.5 months with thermal stability at ≤300°C. This method is amendable for large-area deposition, large-scale manufacturing, and ultimately leads to energy-efficient, low-cost, and stable optoelectronics.
Research Organization:
Argonne National Laboratory (ANL)
Sponsoring Organization:
USDOE Office of Science - Office of Basic Energy Sciences - Materials Sciences and Engineering Division; USDOE Office of Science - Office of Basic Energy Sciences
DOE Contract Number:
AC02-06CH11357
OSTI ID:
1459869
Journal Information:
Advanced Energy Materials, Journal Name: Advanced Energy Materials Journal Issue: 5 Vol. 8; ISSN 1614-6832
Publisher:
Wiley
Country of Publication:
United States
Language:
English

References (58)

GSAS-II : the genesis of a modern open-source all purpose crystallography software package journal March 2013
Stripping down SN2 journal June 2012
Solvent engineering for high-performance inorganic–organic hybrid perovskite solar cells journal July 2014
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) journal January 2015
Enhanced optoelectronic quality of perovskite thin films with hypophosphorous acid for planar heterojunction solar cells journal November 2015
Toward Tailored Film Morphologies: The Origin of Crystal Orientation in Hybrid Perovskite Thin Films journal October 2016
CH 3 NH 3 PbCl 3 Single Crystals: Inverse Temperature Crystallization and Visible-Blind UV-Photodetector journal September 2015
Dielectric Constants of Water, Methanol, Ethanol, Butanol and Acetone: Measurement and Computational Study journal May 2010
Crystal Growth and Dissolution of Methylammonium Lead Iodide Perovskite in Sequential Deposition: Correlation between Morphology Evolution and Photovoltaic Performance journal March 2017
Hysteresis-less inverted CH 3 NH 3 PbI 3 planar perovskite hybrid solar cells with 18.1% power conversion efficiency journal January 2015
Mayer Bond Order as a Metric of Complexation Effectiveness in Lead Halide Perovskite Solutions journal November 2016
Methylammonium lead triiodide perovskite solar cells: A new paradigm in photovoltaics journal August 2015
Development of the Colle-Salvetti correlation-energy formula into a functional of the electron density journal January 1988
Sequential deposition as a route to high-performance perovskite-sensitized solar cells journal July 2013
High-quality bulk hybrid perovskite single crystals within minutes by inverse temperature crystallization journal July 2015
Chemical and Electronic Structure Characterization of Lead Halide Perovskites and Stability Behavior under Different Exposures—A Photoelectron Spectroscopy Investigation journal February 2015
The effects of solvation on the properties of anions in dipolar aprotic solvents journal January 1962
Tracking the formation of methylammonium lead triiodide perovskite journal August 2015
Formation of Thin Films of Organic-Inorganic Perovskites for High-Efficiency Solar Cells journal February 2015
On the Thermal and Thermodynamic (In)Stability of Methylammonium Lead Halide Perovskites journal August 2016
Synthesis and Characterization of Organic−Inorganic Perovskite Thin Films Prepared Using a Versatile Two-Step Dipping Technique journal January 1998
Gas-phase hydration reactions of protonated alcohols. Energetics and bulk hydration of cluster ions journal September 1986
Enhanced Photoluminescence and Solar Cell Performance via Lewis Base Passivation of Organic–Inorganic Lead Halide Perovskites journal September 2014
The role of databases in support of computational chemistry calculations journal October 1996
Reproducible Fabrication of Efficient Perovskite-based Solar Cells: X-ray Crystallographic Studies on the Formation of CH 3 NH 3 PbI 3 Layers journal May 2014
Pathways toward high-performance perovskite solar cells: review of recent advances in organo-metal halide perovskites for photovoltaic applications journal April 2016
Investigation of moisture stability and PL characteristics of terpineol-passivated organic–inorganic hybrid perovskite journal September 2016
Solution Growth of Single Crystal Methylammonium Lead Halide Perovskite Nanostructures for Optoelectronic and Photovoltaic Applications journal April 2015
Relationships between Lead Halide Perovskite Thin-Film Fabrication, Morphology, and Performance in Solar Cells journal November 2015
One-step, low-temperature deposited perovskite solar cell utilizing small molecule additive journal January 2015
Thermal Behavior of Methylammonium Lead-Trihalide Perovskite Photovoltaic Light Harvesters journal October 2014
Ultrasmooth organic–inorganic perovskite thin-film formation and crystallization for efficient planar heterojunction solar cells journal January 2015
A facile solvothermal growth of single crystal mixed halide perovskite CH3NH3Pb(Br1−xClx)3 journal January 2015
Bulk crystal growth of hybrid perovskite material CH 3 NH 3 PbI 3 journal January 2015
Direct Crystallization Route to Methylammonium Lead Iodide Perovskite from an Ionic Liquid journal April 2015
Hydrogen bond network relaxation resolved by alcohol hydration (methanol, ethanol, and glycerol): Alcohol-induced hydrogen-bond network relaxation journal November 2016
Stability of Organic Cations in Solution-Processed CH 3 NH 3 PbI 3 Perovskites: Formation of Modified Surface Layers journal September 2015
Mechanism for rapid growth of organic–inorganic halide perovskite crystals journal November 2016
Impact of Processing Temperature and Composition on the Formation of Methylammonium Lead Iodide Perovskites journal June 2015
Selective dissolution of halide perovskites as a step towards recycling solar cells journal May 2016
Metal halide perovskites for energy applications journal May 2016
Visualizing Carrier Diffusion in Individual Single-Crystal Organolead Halide Perovskite Nanowires and Nanoplates journal September 2015
Organometal Halide Perovskites as Visible-Light Sensitizers for Photovoltaic Cells journal May 2009
Atomistic Origins of High-Performance in Hybrid Halide Perovskite Solar Cells journal April 2014
Towards stable and commercially available perovskite solar cells journal October 2016
Density‐functional thermochemistry. III. The role of exact exchange journal April 1993
Electron-Hole Diffusion Lengths Exceeding 1 Micrometer in an Organometal Trihalide Perovskite Absorber journal October 2013
Dipolar Aprotic Solvents in Bimolecular Aromatic Nucleophilic Substitution Reactions 1 journal January 1961
Solution-Grown Monocrystalline Hybrid Perovskite Films for Hole-Transporter-Free Solar Cells journal March 2016
Persistent Dopants and Phase Segregation in Organolead Mixed-Halide Perovskites journal August 2016
Unreacted PbI 2 as a Double-Edged Sword for Enhancing the Performance of Perovskite Solar Cells journal August 2016
Making and Breaking of Lead Halide Perovskites journal January 2016
Organometal halide perovskite solar cells: degradation and stability journal January 2016
Hydration of methylamine and methylammonium ion: structural and thermodynamic properties from the data of the integral equation method in the RISM approximation journal February 2012
Low trap-state density and long carrier diffusion in organolead trihalide perovskite single crystals journal January 2015
The solubility of some sparingly soluble lead salts: An evaluation of the solubility in water and aqueous electrolyte solution journal July 1980
Improved performance and stability of perovskite solar cells by crystal crosslinking with alkylphosphonic acid ω-ammonium chlorides journal August 2015
Low surface recombination velocity in solution-grown CH3NH3PbBr3 perovskite single crystal journal August 2015

Cited By (5)


Similar Records

Substitutional Growth of Methylammonium Lead Iodide Perovskites in Alcohols
Journal Article · Thu Sep 28 20:00:00 EDT 2017 · Advanced Energy Materials · OSTI ID:1427505

In situ nucleophilic substitutional growth of methylammonium lead iodide polycrystals.
Journal Article · Sat Dec 31 23:00:00 EST 2016 · Nature Chemistry · OSTI ID:1429616

Related Subjects