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Title: Degradation of Highly Alloyed Metal Halide Perovskite Precursor Inks: Mechanism and Storage Solutions

Abstract

Whereas the promise of metal halide perovskite (MHP) photovoltaics (PV) is that they can combine high efficiency with solution-processability, the chemistry occurring in precursor inks is largely unexplored. Herein, we investigate the degradation of MHP solutions based on the most widely used solvents, dimethylformamide (DMF) and dimethyl sulfoxide (DMSO). For the MHP inks studied, which contain formamidinium (FA+), methylammonium (MA+), cesium (Cs+), lead (Pb2+), bromide (Br-), and iodide (I-), dramatic compositional changes are observed following storage of the inks in nitrogen in the dark. We show that hydrolysis of DMF in the precursor solution forms dimethylammonium formate, which subsequently incorporates into the MHP film to compromise the ability of Cs+ and MA+ to stabilize FA+-based MHP. The changes in solution chemistry lead to a modification of the perovskite film stoichiometry, band gap, and structure. The solid precursor salts are stable when ball-milled into a powder, allowing for the storage of large quantities of stoichiometric precursor materials.

Authors:
 [1];  [2];  [2];  [2];  [2];  [2];  [3];  [3];  [2]
  1. National Renewable Energy Lab. (NREL), Golden, CO (United States); Univ. of Colorado, Boulder, CO (United States)
  2. National Renewable Energy Lab. (NREL), Golden, CO (United States)
  3. Univ. of Colorado, Boulder, CO (United States)
Publication Date:
Research Org.:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Solar Energy Technologies Office (EE-4S); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1432603
Report Number(s):
NREL/JA-5K00-71274
Journal ID: ISSN 2380-8195
Grant/Contract Number:
AC36-08GO28308
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
ACS Energy Letters
Additional Journal Information:
Journal Volume: 3; Journal Issue: 4; Journal ID: ISSN 2380-8195
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
14 SOLAR ENERGY; 36 MATERIALS SCIENCE; metal halide perovskite; photovoltaics; degradation; efficiency

Citation Formats

Dou, Benjia, Wheeler, Lance M., Christians, Jeffrey A., Moore, David. T., Harvey, Steven P., Berry, Joseph J., Barnes, Frank S., Shaheen, Sean. E., and van Hest, Maikel F. A. M. Degradation of Highly Alloyed Metal Halide Perovskite Precursor Inks: Mechanism and Storage Solutions. United States: N. p., 2018. Web. doi:10.1021/acsenergylett.8b00305.
Dou, Benjia, Wheeler, Lance M., Christians, Jeffrey A., Moore, David. T., Harvey, Steven P., Berry, Joseph J., Barnes, Frank S., Shaheen, Sean. E., & van Hest, Maikel F. A. M. Degradation of Highly Alloyed Metal Halide Perovskite Precursor Inks: Mechanism and Storage Solutions. United States. doi:10.1021/acsenergylett.8b00305.
Dou, Benjia, Wheeler, Lance M., Christians, Jeffrey A., Moore, David. T., Harvey, Steven P., Berry, Joseph J., Barnes, Frank S., Shaheen, Sean. E., and van Hest, Maikel F. A. M. Wed . "Degradation of Highly Alloyed Metal Halide Perovskite Precursor Inks: Mechanism and Storage Solutions". United States. doi:10.1021/acsenergylett.8b00305.
@article{osti_1432603,
title = {Degradation of Highly Alloyed Metal Halide Perovskite Precursor Inks: Mechanism and Storage Solutions},
author = {Dou, Benjia and Wheeler, Lance M. and Christians, Jeffrey A. and Moore, David. T. and Harvey, Steven P. and Berry, Joseph J. and Barnes, Frank S. and Shaheen, Sean. E. and van Hest, Maikel F. A. M.},
abstractNote = {Whereas the promise of metal halide perovskite (MHP) photovoltaics (PV) is that they can combine high efficiency with solution-processability, the chemistry occurring in precursor inks is largely unexplored. Herein, we investigate the degradation of MHP solutions based on the most widely used solvents, dimethylformamide (DMF) and dimethyl sulfoxide (DMSO). For the MHP inks studied, which contain formamidinium (FA+), methylammonium (MA+), cesium (Cs+), lead (Pb2+), bromide (Br-), and iodide (I-), dramatic compositional changes are observed following storage of the inks in nitrogen in the dark. We show that hydrolysis of DMF in the precursor solution forms dimethylammonium formate, which subsequently incorporates into the MHP film to compromise the ability of Cs+ and MA+ to stabilize FA+-based MHP. The changes in solution chemistry lead to a modification of the perovskite film stoichiometry, band gap, and structure. The solid precursor salts are stable when ball-milled into a powder, allowing for the storage of large quantities of stoichiometric precursor materials.},
doi = {10.1021/acsenergylett.8b00305},
journal = {ACS Energy Letters},
number = 4,
volume = 3,
place = {United States},
year = {Wed Mar 14 00:00:00 EDT 2018},
month = {Wed Mar 14 00:00:00 EDT 2018}
}

Journal Article:
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