Direct calorimetric verification of thermodynamic instability of lead halide hybrid perovskites

Nagabhushana, G. P.; Shivaramaiah, Radha; Navrotsky, Alexandra

doi:10.1073/pnas.1607850113

Title: Direct calorimetric verification of thermodynamic instability of lead halide hybrid perovskites

Abstract

Hybrid perovskites, especially methylammonium lead iodide (MAPbI₃), exhibit excellent solar power conversion efficiencies. However, their application is plagued by poor chemical and structural stability. In this paper, using direct calorimetric measurement of heats of formation, MAPbI₃ is shown to be thermodynamically unstable with respect to decomposition to lead iodide and methylammonium iodide, even in the absence of ambient air or light or heat-induced defects, thus limiting its long-term use in devices. The formation enthalpy from binary halide components becomes less favorable in the order MAPbCl₃, MAPbBr₃, MAPbI₃, with only the chloride having a negative heat of formation. Finally, optimizing the geometric match of constituents as measured by the Goldschmidt tolerance factor provides a potentially quantifiable thermodynamic guide for seeking chemical substitutions to enhance stability.

Authors:

Nagabhushana, G. P. ^[1]; Shivaramaiah, Radha ^[1]; Navrotsky, Alexandra ^[1]

Peter A. Rock Thermochemistry Laboratory and Nanomaterials in the Environment, Agriculture, and Technology Organized Research Unit, University of California, Davis, CA 95616

Publication Date:: Tue Jun 28 00:00:00 EDT 2016

Research Org.:: Univ. of California, Davis, CA (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:: 1259914

Alternate Identifier(s):: OSTI ID: 1470072

Grant/Contract Number:: FG02-03ER46053

Resource Type:: Published Article

Journal Name:: Proceedings of the National Academy of Sciences of the United States of America

Additional Journal Information:: Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Volume: 113 Journal Issue: 28; Journal ID: ISSN 0027-8424

Publisher:: Proceedings of the National Academy of Sciences

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE; hybrid halide perovskites; thermodynamic instability; solar cells; tolerance factor; enthalpy of formation

Citation Formats


                    Nagabhushana, G. P., Shivaramaiah, Radha, and Navrotsky, Alexandra. Direct calorimetric verification of thermodynamic instability of lead halide hybrid perovskites.  United States: N. p., 2016. 
Web.  doi:10.1073/pnas.1607850113.

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                    Nagabhushana, G. P., Shivaramaiah, Radha, & Navrotsky, Alexandra. Direct calorimetric verification of thermodynamic instability of lead halide hybrid perovskites.  United States.  https://doi.org/10.1073/pnas.1607850113

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                    Nagabhushana, G. P., Shivaramaiah, Radha, and Navrotsky, Alexandra. Tue .  
"Direct calorimetric verification of thermodynamic instability of lead halide hybrid perovskites".  United States.  https://doi.org/10.1073/pnas.1607850113.

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@article{osti_1259914,

  title        = {Direct calorimetric verification of thermodynamic instability of lead halide hybrid perovskites},

  author       = {Nagabhushana, G. P. and Shivaramaiah, Radha and Navrotsky, Alexandra},

  abstractNote = {Hybrid perovskites, especially methylammonium lead iodide (MAPbI3), exhibit excellent solar power conversion efficiencies. However, their application is plagued by poor chemical and structural stability. In this paper, using direct calorimetric measurement of heats of formation, MAPbI3 is shown to be thermodynamically unstable with respect to decomposition to lead iodide and methylammonium iodide, even in the absence of ambient air or light or heat-induced defects, thus limiting its long-term use in devices. The formation enthalpy from binary halide components becomes less favorable in the order MAPbCl3, MAPbBr3, MAPbI3, with only the chloride having a negative heat of formation. Finally, optimizing the geometric match of constituents as measured by the Goldschmidt tolerance factor provides a potentially quantifiable thermodynamic guide for seeking chemical substitutions to enhance stability.},

  doi          = {10.1073/pnas.1607850113},

  journal      = {Proceedings of the National Academy of Sciences of the United States of America},

  number       = 28,

  volume       = 113,

  place        = {United States},

  year         = {Tue Jun 28 00:00:00 EDT 2016},

  month        = {Tue Jun 28 00:00:00 EDT 2016}

}

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Title: Direct calorimetric verification of thermodynamic instability of lead halide hybrid perovskites

Abstract

Citation Formats

Dynamic disorder in methylammoniumtrihalogenoplumbates (II) observed by millimeter‐wave spectroscopy journal, December 1987

MOF-5: Enthalpy of Formation and Energy Landscape of Porous Materials journal, June 2011

Solar cell efficiency tables (version 42): Solar cell efficiency tables journal, July 2013

Bandgap calculations and trends of organometal halide perovskites journal, August 2014

Sequential deposition as a route to high-performance perovskite-sensitized solar cells journal, July 2013

Stability Issues on Perovskite Solar Cells journal, November 2015

Organometal Halide Perovskites as Visible-Light Sensitizers for Photovoltaic Cells journal, May 2009

Efficient photodiodes from interpenetrating polymer networks journal, August 1995

Die Gesetze der Krystallochemie journal, May 1926

Solid-state principles applied to organic–inorganic perovskites: new tricks for an old dog journal, January 2014

Intrinsic Thermal Instability of Methylammonium Lead Trihalide Perovskite journal, June 2015

Cesium Enhances Long-Term Stability of Lead Bromide Perovskite-Based Solar Cells journal, December 2015

Thermochemistry of Multiferroic Organic–Inorganic Hybrid Perovskites [(CH 3 ) 2 NH 2 ][M(HCOO) 3 ] (M = Mn, Co, Ni, and Zn) journal, August 2015

Formamidinium lead trihalide: a broadly tunable perovskite for efficient planar heterojunction solar cells journal, January 2014

CH3NH3SnBrxI3-x (x = 0-3), ein Sn(II)-System mit kubischer Perowskitstruktur / CH3NH3SnBrxI3-x(x = 0-3), a Sn(II)-System with Cubic Perovskite Structure journal, August 1978

Making and Breaking of Lead Halide Perovskites journal, January 2016

Efficient planar heterojunction perovskite solar cells by vapour deposition journal, September 2013

Polymer Photovoltaic Cells: Enhanced Efficiencies via a Network of Internal Donor-Acceptor Heterojunctions journal, December 1995

Efficient Hybrid Solar Cells Based on Meso-Superstructured Organometal Halide Perovskites journal, October 2012

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Standard enthalpies of formation and thermodynamic cycle values of crystal lattice energies of methylammonium halides journal, January 1976

Investigation of CH 3 NH 3 PbI 3 Degradation Rates and Mechanisms in Controlled Humidity Environments Using in Situ Techniques journal, January 2015

Compositional engineering of perovskite materials for high-performance solar cells journal, January 2015

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CH3NH3PbX3, ein Pb(II)-System mit kubischer Perowskitstruktur / CH3NH3PbX3, a Pb(II)-System with Cubic Perovskite Structure journal, December 1978

Influence of halide precursor type and its composition on the electronic properties of vacuum deposited perovskite films journal, January 2015

Enthalpy of formation of zinc acetate dihydrate journal, June 2011

Transformation of the Excited State and Photovoltaic Efficiency of CH 3 NH 3 PbI 3 Perovskite upon Controlled Exposure to Humidified Air journal, January 2015

Hybrid Organic-Inorganic Perovskites (HOIPs): Opportunities and Challenges journal, July 2015

Mechanical properties of organic–inorganic halide perovskites, CH 3 NH 3 PbX 3 (X = I, Br and Cl), by nanoindentation journal, January 2015

Carbon Nanotube/Polymer Composites as a Highly Stable Hole Collection Layer in Perovskite Solar Cells journal, September 2014

Dynamic disorder in methylammoniumtrihalogenoplumbates (II) observed by millimeter‐wave spectroscopy
journal, December 1987

MOF-5: Enthalpy of Formation and Energy Landscape of Porous Materials
journal, June 2011

Solar cell efficiency tables (version 42): Solar cell efficiency tables
journal, July 2013

Bandgap calculations and trends of organometal halide perovskites
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Sequential deposition as a route to high-performance perovskite-sensitized solar cells
journal, July 2013

Stability Issues on Perovskite Solar Cells
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Intrinsic Thermal Instability of Methylammonium Lead Trihalide Perovskite
journal, June 2015

Cesium Enhances Long-Term Stability of Lead Bromide Perovskite-Based Solar Cells
journal, December 2015

Thermochemistry of Multiferroic Organic–Inorganic Hybrid Perovskites [(CH ₃ ) ₂ NH ₂ ][M(HCOO) ₃ ] (M = Mn, Co, Ni, and Zn)
journal, August 2015

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journal, January 2014

CH3NH3SnBrxI3-x (x = 0-3), ein Sn(II)-System mit kubischer Perowskitstruktur / CH3NH3SnBrxI3-x(x = 0-3), a Sn(II)-System with Cubic Perovskite Structure
journal, August 1978

Making and Breaking of Lead Halide Perovskites
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Efficient planar heterojunction perovskite solar cells by vapour deposition
journal, September 2013

Polymer Photovoltaic Cells: Enhanced Efficiencies via a Network of Internal Donor-Acceptor Heterojunctions
journal, December 1995

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journal, October 2012

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journal, April 2012

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journal, August 2012

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journal, February 2014

Standard enthalpies of formation and thermodynamic cycle values of crystal lattice energies of methylammonium halides
journal, January 1976

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journal, January 2015

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journal, January 2015

Halide-Dependent Electronic Structure of Organolead Perovskite Materials
journal, June 2015

CH3NH3PbX3, ein Pb(II)-System mit kubischer Perowskitstruktur / CH3NH3PbX3, a Pb(II)-System with Cubic Perovskite Structure
journal, December 1978

Influence of halide precursor type and its composition on the electronic properties of vacuum deposited perovskite films
journal, January 2015

Enthalpy of formation of zinc acetate dihydrate
journal, June 2011

Transformation of the Excited State and Photovoltaic Efficiency of CH ₃ NH ₃ PbI ₃ Perovskite upon Controlled Exposure to Humidified Air
journal, January 2015

Hybrid Organic-Inorganic Perovskites (HOIPs): Opportunities and Challenges
journal, July 2015

Mechanical properties of organic–inorganic halide perovskites, CH ₃ NH ₃ PbX ₃ (X = I, Br and Cl), by nanoindentation
journal, January 2015

Carbon Nanotube/Polymer Composites as a Highly Stable Hole Collection Layer in Perovskite Solar Cells
journal, September 2014