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Proceeding Paper

Effects of Cesium/Formamidinium Co-Addition to Perovskite Solar Cells †

by
Ren Nonomura
1,
Takeo Oku
1,*,
Iori Ono
1,
Atsushi Suzuki
1,
Masanobu Okita
2,
Sakiko Fukunishi
2,
Tomoharu Tachikawa
2 and
Tomoya Hasegawa
2
1
Department of Materials Science, The University of Shiga Prefecture, 2500 Hassaka, Hikone 522-8533, Shiga, Japan
2
Osaka Gas Chemicals Co., Ltd., 5-11-61 Torishima, Konohana-ku, Osaka Shi 554-0051, Osaka Fu, Japan
*
Author to whom correspondence should be addressed.
†
Presented at the 3rd International Electronic Conference on Applied Sciences, 1–15 December 2022; Available online: https://asec2022.sciforum.net/.
Eng. Proc. 2023, 31(1), 32; https://doi.org/10.3390/ASEC2022-13789
Published: 2 December 2022
(This article belongs to the Proceedings of The 3rd International Electronic Conference on Applied Sciences)
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Versions Notes

Abstract

:
In this study, the stabilities and conversion efficiencies of perovskite solar cells including cesium (Cs) or formamidinium (FA) at the CH₃NH₃ site were investigated. The additive effects on the photovoltaic properties and crystalline structures were investigated via current–voltage measurements, X-ray diffraction, and scanning electron microscopy. The simultaneous co-addition of Cs and FA to the CH3NH3PbI3 perovskite crystal improved the photovoltaic properties, which may be due to the suppression of the decomposition of the perovskite crystals and the promotion of crystal growth.

1. Introduction

The recently developed CH3NH3PbI3 (MAPbI3) perovskite solar cells have several advantages, such as tunable band gaps, easy fabrication processes, and high conversion efficiencies [1,2,3,4,5]. However, MAPbI3 is typically unstable in air because of the migration of CH3NH3 (MA). Therefore, the stability of perovskite solar cells should be improved, and one method to improve the stability is elemental adding to perovskite compounds [5,6,7].
Formamidinium (CH(NH2)2, FA) has a larger ionic radius (2.53 Å) than MA (2.17 Å), and it can be expected to improve the structural stability [5]. Several studies on FA addition have been carried out, and the photovoltaic properties and stability of MAPbI3 have been improved [8,9,10,11]. FA addition is expected to extend the carrier lifetime and to reduce the carrier recombination in perovskite layers. Besides FA addition, various alkali cations and organic molecules, such as cesium (Cs) [12,13,14], rubidium (Rb) [15,16,17,18], potassium (K) [19,20,21,22,23], sodium (Na) [24,25,26,27], guanidinium (C(NH2)3, GA) [28,29,30,31], and ethyl ammonium (CH3CH2NH2, EA) [32,33], have been added to stabilize MAPbI3 perovskite crystals, and the photovoltaic properties have been improved by these additions.
Another approach to improve the stability of perovskite solar cells is the introduction of polysilane materials into perovskite devices [34,35,36]. Polysilanes are p-type semiconductors, which promote hole transfer [37], and polysilanes are more stable than ordinary organic materials at elevated temperatures above 300 °C; they are expected to provide a protective layer when deposited on perovskite compounds [38,39].
The purpose of the present work is to fabricate and characterize perovskite solar cells, in which small amounts of FA and Cs are added to MAPbI3 and annealed at a high temperature of 190 °C in ambient air, and the DPPS layer is applied to the perovskite layer. The annealing temperature is higher than 140 °C, which may lead to the stabilization of the perovskite grains.

2. Experimental Procedures

A schematic illustration showing the fabrication processes used to fabricate photovoltaic cells is shown in Figure 1. All processes were performed in air [40,41] by using the air-blow method, and the details are described in previous papers [42,43]. Standard MAPbI3 precursors with molar concentrations of MAI and PbCl2 of 2.4 and 0.8 M, respectively, were prepared, and FAI- and CsI-added precursors were also prepared. To stabilize the perovskite structure, FA and Cs were co-added to the crystals. The DPPS solutions were prepared from decaphenylcyclopentasilane (SI-30-15, Osaka Gas Chemical, Osaka, Japan) and chlorobenzene [38].

3. Results and Discussion

The photovoltaic properties of the present perovskite solar cells were investigated using J-V curves obtained under illumination, as shown in Figure 2a. The photovoltaic parameters, namely, short-circuit current densities (JSC), open-circuit voltages (VOC), the fill factor (FF), the series resistance (Rs), the shunt resistance (Rsh), the photoconversion efficiency (η), the averaged photoconversion efficiency (ηave), and the energy gap (Eg) of all analyzed cells are listed in Table 1. The JSC and η values increased by adding FA and Cs. The EQE values of the present devices that contained FAI and CsI are shown in Figure 2b. The energy gaps were calculated from the EQE spectra, and they are listed in Table 1. The Eg values of the Cs-added perovskites were higher than those of the standard MAPbI3.
The XRD patterns and lattice constants of the perovskite compound in the present devices are shown in Figure 3 and Table 2, respectively. The intensity of the 100 peak for the FAI 25%- and CsI 3%-added device increased, and the crystal orientation of the I100/I210 ratio increased from 3.0 to 9.7, as listed in Table 2. This indicates the crystal growth of (100)-oriented perovskite grains, and the addition of small amounts of FA and Cs improved the crystal orientation and suppressed the grain boundaries in the perovskite layer. The crystal growth in the perovskite layer may reduce the trap density between the perovskite grains and increase the JSC and η.
The elemental mappings arising from the Cs K, Pb M, I L, Cl K, C K, and N K lines are shown for the corresponding SEM images of the present perovskite solar cells, as shown in Figure 4. Compositions of the perovskites in the solar cells are summarized in Table 3. The perovskite particles with smaller sizes were distributed densely for the FAI- and CsI-added devices, each element was distributed homogeneously in the perovskite layer, and Cs atoms were also distributed in the perovskite layer. The elemental composition of Cl increased due to the FA and Cs addition.
The changes in the η of the perovskite solar cells were investigated at 25 °C and 20% humidity for 42 days, as shown in Figure 5a. For the standard MAPbI3 solar cell, η decreased after 14 days. This degradation may be due to the decrease in the photo-current caused by carrier recombination around the defects that formed due to the diffusion of MA cations and halogen anions over the long-term period. The η decrease was mitigated by the FA and Cs addition.
An energy level diagram of the cells is presented in Figure 5b. The previously reported values were also used for the energy levels. The electronic charge generation is caused by light irradiation from the FTO substrate side. The TiO2 layer receives the electrons from the perovskite crystal, and the electrons are transported to the FTO. The holes are transported to a Au electrode through spiro-OMeTAD.

4. Conclusions

The stabilities and conversion efficiencies of the perovskite solar cells were improved by incorporating Cs or FA at the CH₃NH₃ site. The additive effects on the photovoltaic properties and crystalline structures were investigated using J-V curves, XRD, and SEM. The simultaneous co-addition of Cs and FA to the CH3NH3PbI3 perovskite crystal improved the photovoltaic properties, which may be due to the suppression of the decomposition of the perovskite crystals and the improvement of carrier transport.

Author Contributions

Conceptualization, R.N., T.O. and I.O.; Methodology, R.N., T.O., I.O. and A.S.; Formal Analysis, R.N., T.O., I.O. and A.S.; Investigation, R.N., T.O., I.O. and A.S.; Resources, M.O., S.F., T.T. and T.H.; Data Curation, R.N., T.O. and I.O.; Writing—Original Draft Preparation, T.O.; Writing—Review and Editing, R.N., T.O., I.O., A.S., M.O., S.F., T.T. and T.H.; Project Administration, T.O.; Funding Acquisition, T.O. All authors have read and agreed to the published version of the manuscript.

Funding

This research was partly funded by the Japan Society for the promotion of Science as a Grant-in-Aid for Scientific Research (C) 21K04809.

Institutional Review Board Statement

Not applicable.

Informed Consent Statement

Not applicable.

Data Availability Statement

Data are contained within the article.

Acknowledgments

The authors would like to acknowledge Takahiro Kamo, Daiichi Kigenso Kagaku Kogyo Co., Ltd, for providing Cs compounds.

Conflicts of Interest

The authors declare no conflict of interest.

References

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Engproc 31 00032 g001 550
Figure 1. Schematic illustration of the fabrication process of the present photovoltaic cells.
Figure 1. Schematic illustration of the fabrication process of the present photovoltaic cells.
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Figure 2. (a) J-V characteristics and (b) EQE of perovskite solar cells that contained FAI- and CsI-added perovskite.
Figure 2. (a) J-V characteristics and (b) EQE of perovskite solar cells that contained FAI- and CsI-added perovskite.
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Figure 3. X-ray diffraction patterns of the present perovskite solar cells.
Figure 3. X-ray diffraction patterns of the present perovskite solar cells.
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Figure 4. SEM images and corresponding elemental mappings of the present devices.
Figure 4. SEM images and corresponding elemental mappings of the present devices.
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Figure 5. (a) Changes in efficiencies. (b) Energy level diagram.
Figure 5. (a) Changes in efficiencies. (b) Energy level diagram.
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Table
Table 1. Measured photovoltaic parameters of the present perovskite solar cells.
Table 1. Measured photovoltaic parameters of the present perovskite solar cells.
DeviceJSC
(mA cm−2)		VOC
(V)		FFRS
(Ω cm2)		RSh
(Ω cm2)		η
(%)		ηave
(%)		Eg
(eV)
FAI (%)CsI (%)
0010.550.7440.5851.493254.594.171.544
12.51.53.840.5130.3642.262240.720.611.554
12.5211.520.6980.6231.9082005.004.301.563
251.512.410.7010.5871.6826545.114.771.549
25214.410.7370.6341.7110,3386.736.381.548
Table
Table 2. Structural parameters of perovskite crystals with added FAI and CsCI.
Table 2. Structural parameters of perovskite crystals with added FAI and CsCI.
DeviceLattice Constant
(Å)		Crystallite Size
(Å)		Orientation
I100/I210
FAI (%)CsCI (%)CsI (%)
0006.279(2)5902.99
12.5006.278(2)6712.62
12.5306.272(2)6319.67
25006.299(1)5793.84
25306.286(1)8763.81
12.501.56.290(3)5454.46
12.5026.282(0)7625.16
2501.56.299(2)5923.05
25026.297(1)6574.46
Table
Table 3. Compositions of the perovskites as measured using EDS.
Table 3. Compositions of the perovskites as measured using EDS.
DevicePb (at%)I (at%)Cl (at%)C:N (at%)
FAI (%)CsCl (%)
0030.357.012.738.6:61.4
12.5029.757.712.748.3:51.7
12.5339.432.128.433.7:66.3
25030.059.110.944.8:55.2
25327.463.09.5736.6:63.4
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MDPI and ACS Style

Nonomura, R.; Oku, T.; Ono, I.; Suzuki, A.; Okita, M.; Fukunishi, S.; Tachikawa, T.; Hasegawa, T. Effects of Cesium/Formamidinium Co-Addition to Perovskite Solar Cells. Eng. Proc. 2023, 31, 32. https://doi.org/10.3390/ASEC2022-13789

AMA Style

Nonomura R, Oku T, Ono I, Suzuki A, Okita M, Fukunishi S, Tachikawa T, Hasegawa T. Effects of Cesium/Formamidinium Co-Addition to Perovskite Solar Cells. Engineering Proceedings. 2023; 31(1):32. https://doi.org/10.3390/ASEC2022-13789

Chicago/Turabian Style

Nonomura, Ren, Takeo Oku, Iori Ono, Atsushi Suzuki, Masanobu Okita, Sakiko Fukunishi, Tomoharu Tachikawa, and Tomoya Hasegawa. 2023. "Effects of Cesium/Formamidinium Co-Addition to Perovskite Solar Cells" Engineering Proceedings 31, no. 1: 32. https://doi.org/10.3390/ASEC2022-13789

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