Ethylenediammonium-Based "hollow" Pb/Sn Perovskites with Ideal Band Gap Yield Solar Cells with Higher Efficiency and Stability

Weijun Ke, Ioannis Spanopoulos, Qing Tu, Ido Hadar, Xiaotong Li, Gajendra S. Shekhawat, Vinayak P. Dravid, Mercouri G Kanatzidis

Research output: Contribution to journalArticle

Abstract

The power conversion efficiency (PCE) of halide perovskite solar cells is now comparable to that of commercial solar cells. These solar cells are generally based on multication mixed-halide perovskite absorbers with nonideal band gaps of 1.5-1.6 eV. The PCE should be able to rise further if the solar cells could use narrower-band gap absorbers (1.2-1.4 eV). Reducing the Pb content of the semiconductors without sacrificing performance is also a significant driver in the perovskite solar cell research. Here, we demonstrate that mixed Pb/Sn-based perovskites containing the oversized ethylenediammonium (en) dication, {en}FA0.5MA0.5Sn0.5Pb0.5I3 (FA = formamidinium, MA = methylammonium), can exhibit ideal band gaps of 1.27-1.38 eV, suitable for the assembly of single-junction solar cells with higher efficiencies. The use of en dication creates a three-dimensional (3D) hollow inorganic perovskite structure, which was verified through crystal density measurements and single-crystal X-ray diffraction structural analysis as well as nuclear magnetic resonance measurements. The {en}FA0.5MA0.5Sn0.5Pb0.5I3 structure has massive Pb/Sn vacancies and much higher chemical stability than the same structure without en and vacancies. This new property reduces the dark current and carrier trap density and increases the carrier lifetime of the Pb/Sn-based perovskite films. Therefore, solar cells using {en}FA0.5MA0.5Sn0.5Pb0.5I3 light absorbers have substantially enhanced air stability and around 20% improvement in efficiency. After overlaying a thin MABr top layer, we found that the {5% en}FA0.5MA0.5Sn0.5Pb0.5I3 material gives an optimized PCE of 17.04%. The results highlight the strong promise of 3D hollow mixed Pb/Sn perovskites in achieving ideal band gap materials with higher chemical stability and lower Pb content for high-performance single-junction solar cells or multijunction solar cells serving as bottom cells.

Original languageEnglish
Pages (from-to)8627-8637
Number of pages11
JournalJournal of the American Chemical Society
Volume141
Issue number21
DOIs
Publication statusPublished - May 29 2019

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Solar cells
Energy gap
Perovskite
Conversion efficiency
Chemical stability
Vacancies
Intercellular Junctions
Magnetic resonance measurement
Carrier lifetime
Dark currents
Structural analysis
Semiconductors
Nuclear magnetic resonance
X-Ray Diffraction
Single crystals
Semiconductor materials
X ray diffraction
Crystals
Magnetic Resonance Spectroscopy
Air

ASJC Scopus subject areas

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

Cite this

Ethylenediammonium-Based "hollow" Pb/Sn Perovskites with Ideal Band Gap Yield Solar Cells with Higher Efficiency and Stability. / Ke, Weijun; Spanopoulos, Ioannis; Tu, Qing; Hadar, Ido; Li, Xiaotong; Shekhawat, Gajendra S.; Dravid, Vinayak P.; Kanatzidis, Mercouri G.

In: Journal of the American Chemical Society, Vol. 141, No. 21, 29.05.2019, p. 8627-8637.

Research output: Contribution to journalArticle

Ke, Weijun ; Spanopoulos, Ioannis ; Tu, Qing ; Hadar, Ido ; Li, Xiaotong ; Shekhawat, Gajendra S. ; Dravid, Vinayak P. ; Kanatzidis, Mercouri G. / Ethylenediammonium-Based "hollow" Pb/Sn Perovskites with Ideal Band Gap Yield Solar Cells with Higher Efficiency and Stability. In: Journal of the American Chemical Society. 2019 ; Vol. 141, No. 21. pp. 8627-8637.
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abstract = "The power conversion efficiency (PCE) of halide perovskite solar cells is now comparable to that of commercial solar cells. These solar cells are generally based on multication mixed-halide perovskite absorbers with nonideal band gaps of 1.5-1.6 eV. The PCE should be able to rise further if the solar cells could use narrower-band gap absorbers (1.2-1.4 eV). Reducing the Pb content of the semiconductors without sacrificing performance is also a significant driver in the perovskite solar cell research. Here, we demonstrate that mixed Pb/Sn-based perovskites containing the oversized ethylenediammonium (en) dication, {en}FA0.5MA0.5Sn0.5Pb0.5I3 (FA = formamidinium, MA = methylammonium), can exhibit ideal band gaps of 1.27-1.38 eV, suitable for the assembly of single-junction solar cells with higher efficiencies. The use of en dication creates a three-dimensional (3D) hollow inorganic perovskite structure, which was verified through crystal density measurements and single-crystal X-ray diffraction structural analysis as well as nuclear magnetic resonance measurements. The {en}FA0.5MA0.5Sn0.5Pb0.5I3 structure has massive Pb/Sn vacancies and much higher chemical stability than the same structure without en and vacancies. This new property reduces the dark current and carrier trap density and increases the carrier lifetime of the Pb/Sn-based perovskite films. Therefore, solar cells using {en}FA0.5MA0.5Sn0.5Pb0.5I3 light absorbers have substantially enhanced air stability and around 20{\%} improvement in efficiency. After overlaying a thin MABr top layer, we found that the {5{\%} en}FA0.5MA0.5Sn0.5Pb0.5I3 material gives an optimized PCE of 17.04{\%}. The results highlight the strong promise of 3D hollow mixed Pb/Sn perovskites in achieving ideal band gap materials with higher chemical stability and lower Pb content for high-performance single-junction solar cells or multijunction solar cells serving as bottom cells.",
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