Critical Role of Water in Defect Aggregation and Chemical Degradation of Perovskite Solar Cells

Yun Hyok Kye, Chol Jun Yu, Un Gi Jong, Yue Chen, Aron Walsh

Research output: Contribution to journalArticle

27 Citations (Scopus)

Abstract

The chemical stability of methylammonium lead iodide (MAPbI3) under humid conditions remains the primary challenge facing halide perovskite solar cells. We investigate defect processes in the water-intercalated iodide perovskite (MAPbI3-H2O) and monohydrated phase (MAPbI3·H2O) within a first-principles thermodynamic framework. We consider the formation energies of isolated and aggregated vacancy defects with different charge states under I-rich and I-poor conditions. It is found that a PbI2 (partial Schottky) vacancy complex can be formed readily, while the MAI vacancy complex is difficult to form in the hydrous compounds. Vacancies in the hydrous phases create deep charge transition levels, indicating the degradation of the lead halide perovskite upon exposure to moisture. Electronic structure analysis supports a mechanism of water-mediated vacancy pair formation.

Original languageEnglish
Pages (from-to)2196-2201
Number of pages6
JournalJournal of Physical Chemistry Letters
Volume9
Issue number9
DOIs
Publication statusPublished - 2018 May 3

Fingerprint

Vacancies
Agglomeration
solar cells
degradation
Degradation
Defects
Water
defects
water
Iodides
Perovskite
iodides
halides
Lead
Chemical stability
energy of formation
moisture
Electronic structure
Moisture
Perovskite solar cells

All Science Journal Classification (ASJC) codes

  • Materials Science(all)
  • Physical and Theoretical Chemistry

Cite this

Kye, Yun Hyok ; Yu, Chol Jun ; Jong, Un Gi ; Chen, Yue ; Walsh, Aron. / Critical Role of Water in Defect Aggregation and Chemical Degradation of Perovskite Solar Cells. In: Journal of Physical Chemistry Letters. 2018 ; Vol. 9, No. 9. pp. 2196-2201.
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Critical Role of Water in Defect Aggregation and Chemical Degradation of Perovskite Solar Cells. / Kye, Yun Hyok; Yu, Chol Jun; Jong, Un Gi; Chen, Yue; Walsh, Aron.

In: Journal of Physical Chemistry Letters, Vol. 9, No. 9, 03.05.2018, p. 2196-2201.

Research output: Contribution to journalArticle

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AU - Walsh, Aron

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AB - The chemical stability of methylammonium lead iodide (MAPbI3) under humid conditions remains the primary challenge facing halide perovskite solar cells. We investigate defect processes in the water-intercalated iodide perovskite (MAPbI3-H2O) and monohydrated phase (MAPbI3·H2O) within a first-principles thermodynamic framework. We consider the formation energies of isolated and aggregated vacancy defects with different charge states under I-rich and I-poor conditions. It is found that a PbI2 (partial Schottky) vacancy complex can be formed readily, while the MAI vacancy complex is difficult to form in the hydrous compounds. Vacancies in the hydrous phases create deep charge transition levels, indicating the degradation of the lead halide perovskite upon exposure to moisture. Electronic structure analysis supports a mechanism of water-mediated vacancy pair formation.

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