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Title: Enhanced Charge Transport in 2D Perovskites via Fluorination of Organic Cation

Abstract

Organic-inorganic halide perovskites incorporating two-dimensional (2D) structures have shown promise for enhancing the stability of perovskite solar cells (PSCs). However, the bulky spacer cations often limit charge transport. Here, we report on a simple approach based on molecular design of the organic spacer to improve the transport properties of 2D perovskites, and we use phenethylammonium (PEA) as an example. We demonstrate that by fluorine substitution on the para position in PEA to form 4-fluorophenethylammonium (F-PEA), the average phenyl ring centroid-centroid distances in the organic layer become shorter with better aligned stacking of perovskite sheets. The impact is enhanced orbital interactions and charge transport across adjacent inorganic layers as well as increased carrier lifetime and reduced trap density. Using a simple perovskite deposition at room temperature without using any additives, we obtained a power conversion efficiency of >13% for (F-PEA) 2MA 4Pb 5I 16-based PSCs. In addition, the thermal stability of 2D PSCs based on F-PEA is significantly enhanced compared to those based on PEA.

Authors:
ORCiD logo [1];  [1]; ORCiD logo [1];  [2];  [1];  [3]; ORCiD logo [1];  [1];  [4]; ORCiD logo [1];  [1]; ORCiD logo [1];  [1];  [3]; ORCiD logo [5]; ORCiD logo [1]; ORCiD logo [1]
  1. National Renewable Energy Lab. (NREL), Golden, CO (United States)
  2. Imperial College, London (United Kingdom)
  3. Univ. of North Carolina, Chapel Hill, NC (United States)
  4. National Renewable Energy Lab. (NREL), Golden, CO (United States); Univ. of Colorado, Boulder, CO (United States)
  5. Imperial College, London (United Kingdom); Yonsei Univ., Seoul (Korea, Republic of)
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:
1506616
Report Number(s):
NREL/JA-5900-73083
Journal ID: ISSN 0002-7863
Grant/Contract Number:  
AC36-08GO28308
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 141; Journal Issue: 14; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
14 SOLAR ENERGY; 36 MATERIALS SCIENCE; perovskites; 2D structures; perovskite solar cells; transport properties

Citation Formats

Zhang, Fei, Kim, Dong Hoe, Lu, Haipeng, Park, Ji-Sang, Larson, Bryon W., Hu, Jun, Gao, Liguo, Xiao, Chuanxiao, Reid, Obadiah G., Chen, Xihan, Zhao, Qian, Ndione, Paul F., Berry, Joseph J., You, Wei, Walsh, Aron, Beard, Matthew C., and Zhu, Kai. Enhanced Charge Transport in 2D Perovskites via Fluorination of Organic Cation. United States: N. p., 2019. Web. doi:10.1021/jacs.9b00972.
Zhang, Fei, Kim, Dong Hoe, Lu, Haipeng, Park, Ji-Sang, Larson, Bryon W., Hu, Jun, Gao, Liguo, Xiao, Chuanxiao, Reid, Obadiah G., Chen, Xihan, Zhao, Qian, Ndione, Paul F., Berry, Joseph J., You, Wei, Walsh, Aron, Beard, Matthew C., & Zhu, Kai. Enhanced Charge Transport in 2D Perovskites via Fluorination of Organic Cation. United States. doi:10.1021/jacs.9b00972.
Zhang, Fei, Kim, Dong Hoe, Lu, Haipeng, Park, Ji-Sang, Larson, Bryon W., Hu, Jun, Gao, Liguo, Xiao, Chuanxiao, Reid, Obadiah G., Chen, Xihan, Zhao, Qian, Ndione, Paul F., Berry, Joseph J., You, Wei, Walsh, Aron, Beard, Matthew C., and Zhu, Kai. Mon . "Enhanced Charge Transport in 2D Perovskites via Fluorination of Organic Cation". United States. doi:10.1021/jacs.9b00972.
@article{osti_1506616,
title = {Enhanced Charge Transport in 2D Perovskites via Fluorination of Organic Cation},
author = {Zhang, Fei and Kim, Dong Hoe and Lu, Haipeng and Park, Ji-Sang and Larson, Bryon W. and Hu, Jun and Gao, Liguo and Xiao, Chuanxiao and Reid, Obadiah G. and Chen, Xihan and Zhao, Qian and Ndione, Paul F. and Berry, Joseph J. and You, Wei and Walsh, Aron and Beard, Matthew C. and Zhu, Kai},
abstractNote = {Organic-inorganic halide perovskites incorporating two-dimensional (2D) structures have shown promise for enhancing the stability of perovskite solar cells (PSCs). However, the bulky spacer cations often limit charge transport. Here, we report on a simple approach based on molecular design of the organic spacer to improve the transport properties of 2D perovskites, and we use phenethylammonium (PEA) as an example. We demonstrate that by fluorine substitution on the para position in PEA to form 4-fluorophenethylammonium (F-PEA), the average phenyl ring centroid-centroid distances in the organic layer become shorter with better aligned stacking of perovskite sheets. The impact is enhanced orbital interactions and charge transport across adjacent inorganic layers as well as increased carrier lifetime and reduced trap density. Using a simple perovskite deposition at room temperature without using any additives, we obtained a power conversion efficiency of >13% for (F-PEA)2MA4Pb5I16-based PSCs. In addition, the thermal stability of 2D PSCs based on F-PEA is significantly enhanced compared to those based on PEA.},
doi = {10.1021/jacs.9b00972},
journal = {Journal of the American Chemical Society},
number = 14,
volume = 141,
place = {United States},
year = {2019},
month = {3}
}

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This content will become publicly available on March 18, 2020
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