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Proceeding Paper

Effects of Guanidinium and Cesium Addition to CH3NH3PbI3 Perovskite Photovoltaic Devices †

by
Takeo Oku
1,*,
Iori Ono
1,
Shoma Uchiya
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), 35; https://doi.org/10.3390/ASEC2022-13769
Published: 1 December 2022
(This article belongs to the Proceedings of The 3rd International Electronic Conference on Applied Sciences)
Browse Figure
Versions Notes

Abstract

:
CH3NH3PbI3 perovskite compounds are unstable in air due to the migration of CH3NH3. The purpose of the present work is to investigate the effects of addition of guanidinium C(NH2)3 (GA) and cesium (Cs) on CH3NH3PbI3 perovskite solar cells. The addition of GA/Cs and the insertion of decaphenylpentasilane between the perovskite and hole transport layer improved the external quantum efficiency and short-circuit current density, and the conversion efficiencies were stable. First-principles calculations on the density of states and band structures showed reduction in the total energy by the GA addition.

1. Introduction

Although silicon is the most common solar cell material, the fabrication process is expensive. On the other hand, CH3NH3PbI3 (MAPbI3) compounds have been widely used for perovskite solar cells [1,2,3,4,5], and the MAPbI3 perovskite compound have tunable band gaps and easy fabrication process with low cost. However, the MAPbI3 compounds are unstable in the ordinary air due to the migration and desorption of CH3NH3 (MA) molecules [6,7,8,9]. In order to stabilize the perovskite structure, various kinds of cations such as formamidinium (HC(NH2)2, FA) [10,11,12,13,14,15,16], ethylammonium (CH3CH2NH3, EA) [17,18], or guanidinium (C(NH2)3, GA) [19,20], which have larger ionic radii than methylammonium (CH3NH3, MA), have been introduced at the MA site, and the fabricated cells were stable to some extent. Introducing alkali metals such as cesium (Cs) [21,22,23], rubidium (Rb) [24,25,26], potassium (K) [27,28,29,30], and sodium (Na) [31,32,33,34], could also be effective because these metal elements do not desorb from the perovskite crystal.
Another approach to improve the stability of the perovskite solar cells is introducing polymeric materials such as polysilane [35,36,37,38,39]. Polysilanes have two important features that are p-type semiconductors and are stable at elevated temperatures above 300 °C.
The purpose of the present work is to fabricate MAPbI3 perovskite solar cells added with GA and Cs, and to characterize the devices from experiments and first-principle calculation. In the present work, polysilane was also used both for protection of the perovskite layer and for hole transport [35,37].

2. Experimental Procedures

A fabrication process of photovoltaic devices of the present work is same as those of the previous works [40,41,42]. A TiO2 compact layer was formed on the F-doped tin-oxide (FTO) substrates, and a mesoporous TiO2 layer was formed on the compact TiO2 layer. A perovskite layer with desired composition was formed on the mesoporous TiO2 layer, and decaphenylcyclopentasilane (DPPS), which is a one kind of polysilane, was formed on the perovskite layer [35]. A layer of 2,2′,7,7′-tetrakis-(N,N-di(p-methoxyphenyl)amine)-9,9′-spirobifluorene (spiro-OMeTAD) was formed on the DPPS, and then gold (Au) metal electrodes were formed on the spiro-OMeTAD hole transport layer.
The current density voltage characteristics of the fabricated devices were measured under a solar simulating light source operated at 100 mW cm−2. X-ray diffraction was used to investigate the microstructures of the devices, and first-principles calculation was also carried out to estimate the properties of the perovskite crystals [43,44,45].

3. Results and Discussion

In order to estimate the structural stability of perovskite compounds, a tolerance factor (t) is used [5,46,47] using the following equation:
t = r A + r X 2 r B + r X
where rA, rB, and rX are the ionic radii of the A, B, and X ions for ABX3 perovskite structures, respectively [5]. When the t-value is 1, the perovskite compound has a stable crystal structure with cubic symmetry. From the previous experimental studies on perovskite compounds, the perovskite structure could be formed in the range of 0.813 ≤ t ≤ 1.107. Calculated t-factors of perovskite compounds are listed in Table 1. From this calculation, co-addition of GA and Cs could be one of the effective ways to stabilize the MAPbI3 structure.
Figure 1a is a structure model of MA0.75GA0.125 Cs0.125PbI3. MA molecules are substituted by GA and Cs, which are located diagonally. Based on this structure model, the physical properties could be predicted. Figure 1b is an electron diffraction pattern of MA0.75GA0.125 Cs0.125PbI3 calculated along [111]. Although the usual MAPbI3 has 6-fold symmetry from the [111] incidence, the calculated electron diffraction pattern in Figure 1b shows 2-fold symmetry, which is due to the doped Cs and GA. Therefore, the high symmetry dimension of the space group of Pm 3 _ m for MAPbI3 is reduced to lower symmetry.
From the first-principle calculations and experimental evaluations, addition of small amount of GA to MAPbI3 is effective to stabilize the perovskite structure [48,49]. Although the addition of GA expands and distorts the crystal lattice of MAPbI3, Cs would reduce the distortion of the lattice, which could lead to the stability of the perovskite crystal.
For the fabricated device with MA0.845GA0.125Cs0.03PbI3 perovskite compound, the high photoconversion efficiency was obtained, which would be in good agreement with the calculated results. The stability of the device at the room temperature was also good. Although several works on GAPbI3 [50] and CsPbI3 [51,52] compounds have been reported, few works have been reported on the co-addition of GA and Cs to MAPbI3. The present work indicated the effectiveness of the co-addition of GA and Cs to the MAPbI3 on the photovoltaic properties for perovskite solar cells.

4. Conclusions

The effects of addition of guanidinium GA and Cs on MAPbI3 perovskite solar cells were investigated. The co-addition of GA/Cs and the insertion of DPPS between the perovskite and spiro-OMeTAD improved the EQE, and the conversion efficiencies were stable. The calculated electron diffraction pattern of MA0.75GA0.125Cs0.125PbI3 showed reduction in the structural symmetry. First-principles calculations also showed reduction in the total energy by the GA addition, which indicated the stabilization by the addition.

Author Contributions

Conceptualization, T.O., I.O. and S.U.; methodology, T.O., I.O., S.U. and A.S.; formal analysis, T.O., I.O., S.U. and A.S.; investigation, T.O., I.O., S.U. and A.S.; resources, M.O., S.F., T.T. and T.H.; data curation, T.O., I.O. and S.U.; writing—original draft preparation, T.O.; writing—review and editing, T.O., I.O., S.U., 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 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 is contained within the article.

Conflicts of Interest

The authors declare no conflict of interest.

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Engproc 31 00035 g001 550
Figure 1. (a) Structure model and (b) calculated electron diffraction pattern along [111] of MA0.75GA0.125 Cs0.125PbI3.
Figure 1. (a) Structure model and (b) calculated electron diffraction pattern along [111] of MA0.75GA0.125 Cs0.125PbI3.
Engproc 31 00035 g001
Table
Table 1. Calculated t-factors of perovskite compounds.
Table 1. Calculated t-factors of perovskite compounds.
Perovskitet
MAPbI30.912
GAPbI31.039
CsPbI30.851
MA0.75GA0.125Cs0.125PbI30.920
MA0.845GA0.125Cs0.03PbI30.926
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MDPI and ACS Style

Oku, T.; Ono, I.; Uchiya, S.; Suzuki, A.; Okita, M.; Fukunishi, S.; Tachikawa, T.; Hasegawa, T. Effects of Guanidinium and Cesium Addition to CH3NH3PbI3 Perovskite Photovoltaic Devices. Eng. Proc. 2023, 31, 35. https://doi.org/10.3390/ASEC2022-13769

AMA Style

Oku T, Ono I, Uchiya S, Suzuki A, Okita M, Fukunishi S, Tachikawa T, Hasegawa T. Effects of Guanidinium and Cesium Addition to CH3NH3PbI3 Perovskite Photovoltaic Devices. Engineering Proceedings. 2023; 31(1):35. https://doi.org/10.3390/ASEC2022-13769

Chicago/Turabian Style

Oku, Takeo, Iori Ono, Shoma Uchiya, Atsushi Suzuki, Masanobu Okita, Sakiko Fukunishi, Tomoharu Tachikawa, and Tomoya Hasegawa. 2023. "Effects of Guanidinium and Cesium Addition to CH3NH3PbI3 Perovskite Photovoltaic Devices" Engineering Proceedings 31, no. 1: 35. https://doi.org/10.3390/ASEC2022-13769

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