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

Fei Zhang, Dong Hoe Kim, Haipeng Lu, Ji Sang Park, Bryon W. Larson, Jun Hu, Liguo Gao, Chuanxiao Xiao, Obadiah G. Reid, Xihan Chen, Qian Zhao, Paul F. Ndione, Joseph J. Berry, Wei You, Aron Walsh, Matthew C. Beard, Kai Zhu

Research output: Contribution to journalArticle

20 Citations (Scopus)

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)2MA4Pb5I16-based PSCs. In addition, the thermal stability of 2D PSCs based on F-PEA is significantly enhanced compared to those based on PEA.

Original languageEnglish
Pages (from-to)5972-5979
Number of pages8
JournalJournal of the American Chemical Society
Volume141
Issue number14
DOIs
Publication statusPublished - 2019 Apr 10

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Fluorination
Halogenation
Cations
Charge transfer
Positive ions
Perovskite
Carrier lifetime
Fluorine
Transport properties
Conversion efficiency
Thermodynamic stability
Substitution reactions
Hot Temperature
Perovskite solar cells
perovskite
Temperature

All Science Journal Classification (ASJC) codes

  • Catalysis
  • Chemistry(all)
  • Biochemistry
  • Colloid and Surface Chemistry

Cite this

Zhang, F., Kim, D. H., Lu, H., Park, J. S., Larson, B. W., Hu, J., ... Zhu, K. (2019). Enhanced Charge Transport in 2D Perovskites via Fluorination of Organic Cation. Journal of the American Chemical Society, 141(14), 5972-5979. https://doi.org/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. In: Journal of the American Chemical Society. 2019 ; Vol. 141, No. 14. pp. 5972-5979.
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author = "Fei Zhang and Kim, {Dong Hoe} and Haipeng Lu and Park, {Ji Sang} and Larson, {Bryon W.} and Jun Hu and Liguo Gao and Chuanxiao Xiao and Reid, {Obadiah G.} and Xihan Chen and Qian Zhao and Ndione, {Paul F.} and Berry, {Joseph J.} and Wei You and Aron Walsh and Beard, {Matthew C.} and Kai Zhu",
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Zhang, F, Kim, DH, Lu, H, Park, JS, Larson, BW, Hu, J, Gao, L, Xiao, C, Reid, OG, Chen, X, Zhao, Q, Ndione, PF, Berry, JJ, You, W, Walsh, A, Beard, MC & Zhu, K 2019, 'Enhanced Charge Transport in 2D Perovskites via Fluorination of Organic Cation', Journal of the American Chemical Society, vol. 141, no. 14, pp. 5972-5979. https://doi.org/10.1021/jacs.9b00972

Enhanced Charge Transport in 2D Perovskites via Fluorination of Organic Cation. / 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.

In: Journal of the American Chemical Society, Vol. 141, No. 14, 10.04.2019, p. 5972-5979.

Research output: Contribution to journalArticle

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T1 - Enhanced Charge Transport in 2D Perovskites via Fluorination of Organic Cation

AU - Zhang, Fei

AU - Kim, Dong Hoe

AU - Lu, Haipeng

AU - Park, Ji Sang

AU - Larson, Bryon W.

AU - Hu, Jun

AU - Gao, Liguo

AU - Xiao, Chuanxiao

AU - Reid, Obadiah G.

AU - Chen, Xihan

AU - Zhao, Qian

AU - Ndione, Paul F.

AU - Berry, Joseph J.

AU - You, Wei

AU - Walsh, Aron

AU - Beard, Matthew C.

AU - Zhu, Kai

PY - 2019/4/10

Y1 - 2019/4/10

N2 - 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.

AB - 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.

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