The stability of inorganic perovskite solar cells: from materials to devices
doi: 10.1088/2752-5724/acd56c
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Abstract: Inorganic halide perovskite solar cells (IHPSCs) have become one of the most promising research hotspots due to to the excellent light and thermal stabilities of inorganic halide perovskites (IHPs). Despite rapid progress in cell performance in very recent years, the phase instability of IHPs easily occurs, which will remarkably influence the cell efficiency and stability. Much effort has been devoted to solving this issue. In this review, we focus on representative progress in the stability from IHPs to IHPSCs, including (i) a brief introduction of inorganic perovskite materials and devices, (ii) some new additives and fabrication methods, (iii) thermal and light stabilities, (iv) tailoring phase stability, (v) optimization of the stability of inorganic perovskite solar cells and (vi) interfacial engineering for stability enhancement. Finally, perspectives will be given regarding future work on highly efficient and stable IHPSCs. This review aims to provide a thorough understanding of the key influential factors on the stability of materials to highly efficient and stable IHPSCs.
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Figure 1. Crystal structure of a typical black phase ABX3 perovskite. Reproduced from [14] with permission from Springer Nature.
Figure 3. (a) Comparison of the thermal phase relationship of CsPbI3 and the phase behavior of strained CsPbI2.7Br0.3 thin films. From [52], reprinted with permission from AAAS. (b) Crystal structure and relative phase transition process of different phases. From [52], reprinted with permission from AAAS.
Figure 4. (a) Theoretical calculation results of the electronic structure of cubic CsPbBr3, including the density of states and the corresponding contributions of elements to the energy band, as well as the electronic distribution of the maximum value of the valence band and the minimum value of the conduction band [53]. John Wiley & Sons. [© 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim]. (b) Binding energy (top), effective mass (middle), and dielectric constant (bottom) versus band gap. Brown, red, and yellow stars represent the results for CsPbI3, CsPbI2Br and CsPbBr3, respectively. Green spheres indicate another experimental finding. Reprinted with permission from [54]. Copyright (2017) American Chemical Society. CC BY 4.0.
Figure 5. (a) Absorbance spectra for IHP films of different components, CsPb(I1-xBrx)3. Reprinted from [34], Copyright (2018), with permission from Elsevier. (b) Visible light absorption coefficient and two-photon absorption coefficient of CsPbBr3 single crystal (SC) [57]. John Wiley & Sons. [© 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim]. (c) The average diffusion lengths measured in APbBr3 SC and previously published MAPbI3 (left), electron and hole diffusion lengths measured in different perovskite components (right). Reprinted with permission from [56]. Copyright (2017) American Chemical Society.
Figure 6. (a) Schematic diagram of the crystal structure relationship between Pb-perovskites and lead-free perovskite derivatives. (b) Elements of halide double perovskites formed by A2BB3+X6. Reprinted with permission from [63]. Copyright (2016) American Chemical Society.
Figure 7. (a) Varieties of device architectures for PSCs. (b) Efficiency evolution of IHPSCs with different architectures [32, 39, 41, 43, 45, 69, 70, 74-77, 79-81]. (c) Relationship between SQ limit of single junction solar cell and band gap of absorber material. (JSC: short circuit current, VOC: open-circuit voltage, FF: fill factor, Eff.: efficiency).
Figure 8. Illustration of preparing IHP absorption layers by different methods. (a) One-step deposition. Reproduced from [39], with permission from Springer Nature. CC BY 4.0. (b) Multi-step deposition. Reproduced with permission from [87]. Copyright 2018, the Royal Society of Chemistry. (c) Vacuum deposition [90]. John Wiley & Sons. [© 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim].
Figure 9. (a) TGA of MABr, PbBr2, CsBr, MAPbBr3 and CsPbBr3. Reprinted with permission from [93]. Copyright (2016) American Chemical Society. (b) MPP test of the unsealed CsPbI2Br (dark gray line) and MAPbI3 solar cells (magenta line) in a nitrogen glovebox (25 C). Reprinted with permission from [38]. Copyright (2017) American Chemical Society. (c) Ionic conductivity of CsPbI2Br and MAPbI3 film in Au/perovskite/Au lateral structures by cryogenic galvanostatic and current-voltage experiments. Reprinted with permission from [38]. Copyright (2017) American Chemical Society.
Figure 10. (a) Absorbance spectra and photoluminescence spectra for CsPb(IxBr1-x)3 films with varying iodide concentration x’. [36] John Wiley & Sons. [© 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim]. (b) Schematic diagram of Pb2+ partially replaced by various metal ions (doping or alloying) can improve the stability of
-CsPbI3 at room temperature by increasing the tolerance factor, and improve the thermal stability of orthogonal CsPbBr3 by increasing the formation energy. Reprinted with permission from [100]. Copyright (2018) American Chemical Society. (c) Histograms comparing the first-principles calculation results of the formation energy (Eform) changes of each divalent Pb2+ ion in CsPbBr3 nanocrystals when undoped and doped with 2.08 mol% of various metal ions. Reprinted with permission from [100]. Copyright (2018) American Chemical Society. Schematic diagram of reducing grain size (d) nanocrystal. Reprinted from [101], Copyright (2017), with permission from Elsevier. (e) Quantum dots (QDs). Reprinted from [102], Copyright (2018), with permission from Elsevier. (f) 2D perovskite. Reprinted from [34], Copyright (2018), with permission from Elsevier. 
Figure 11. (a) Schematic diagram of the crystallization process of CsPbI2Br perovskite treated with GTA or GTA-ATS; SEM images of corresponding films and stability characterization of the corresponding device. Reprinted from [86], Copyright (2019), with permission from Elsevier. (b) Schematic diagram of the stabilization of
-phase CsPbI3, the histogram of the PCE values corresponding to devices with different crystal phase absorption layers and their stability as a function of storage time. Reprinted with permission from [111]. Copyright (2018) American Chemical Society. (c) Scheme for the perovskite crystal growth and additive volatilization of the film [42]. John Wiley & Sons. [© 2021 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim]. (d) Schematic phase conversion and mechanism for the accelerated crystallization process based on the pristine and molten-salt-assisted crystallization films [112]. John Wiley & Sons. [© 2021 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim]. (e) Photographs of perovskite precursor solutions based on DMAAc and DMF solvents, schematic diagrams of cation/anion/solvent interactions in the solutions and the stability characterization of the corresponding device [46]. John Wiley & Sons. [© 2022 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim]. 
Figure 12. (a) ETL/IHP interface modified by LiF [116]. John Wiley & Sons. [© 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim]. (b) Schematic diagram of 3D CsPbI3 treated with 1D PTAPbI3 and 2D PTA2PbI4 composition at the grain boundaries, and long-term stability testing of unencapsulated devices under ambient conditions [69]. John Wiley & Sons. [© 2022 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim]. (c) Simultaneous modification of ETL/PVSK and PVSK/HTL interfaces [96]. John Wiley & Sons. [© 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim]. (d) CsMX3 perovskite solar cells based on carbon electrode instead of gold electrode. Reprinted with permission from [120]. Copyright (2017) American Chemical Society.
Figure 13. (a) SEM surface images of the CsPbI3 perovskite films, the photographs of a CsPbI3 perovskite minimodule and long-term stability test of an encapsulated CsPbI3 perovskite minimodule under different conditions. Reprinted from [121], Copyright (2022), with permission from Elsevier. (b) Schematic diagram of the device structure with a 2D Cs2PbI2Cl2 layer at the top of the 3D perovskite active layer (left). Accelerated aging of PSCs operating at elevated temperatures (right). Reprinted from [109], with permission from AAAS.
Table 1. Evolution of the device efficiency and stability depending on the components of the absorber material and the device architecture (MPP = maximum power point, RH = relative humidity).
Device architecture Absorber material PCE Stability References n-i-p CsPbI3 21.0% 98% of its initial PCE over 500 h (light intensity = LED illumination (100 mW cm-2), applied bias = 0.85 V, atmosphere = N2 atmosphere). [69] CsPbI3-xBrx 21.8% 89.3% of its original efficiency at 85 C for 120 h (atmosphere = N2 atmosphere). [70] p-i-n CsPbI3 19.84% 95% of its initial efficiency after the same operation for 1000 h (light intensity = LED illumination (100 mW cm-2), applied bias = MPP, atmosphere = N2 atmosphere, temperature 45 C). [74] CsPbI3-xBrx 17.02% 80% of its PCE after 1000 h (light intensity = dark, atmosphere = air atmosphere, RH = 30%). [79] HTM-free CsPbI3 16.7% 80% of their initial PCE at 85 C for 200 h (atmosphere = air atmosphere, temperature = 20 C-30 C, RH = 5%-20%, no encapsulation). [76] CsPbI3-xBrx 14.84% 94% of its initial PCE after storage for 30 d (atmosphere = air atmosphere, temperature = room temperature, RH = 20%-25%). [80] CsPbBr3 11.08% Nearly unchanged over 100 d and 85 C over 30 d (atmosphere = air atmosphere, temperature = 85 C, RH = 40%, no encapsulation). [81] 
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Table 2. Comparison of different inorganic perovskite deposition methods with their stability and best efficiency documented.
Deposition Absorber material PCE Stability References Solution processing One-step spin-coating CsPbI3-xBrx 21.8% 89.3% of its original efficiency at 85 C for 120 h (N2 atmosphere). [70] Two-step spin-coating CsPbI3-xBrx 12.5% 98% of the initial PCE for 480 h (stored under ambient conditions without encapsulation). [87] Vacuum deposition processing CsPbI2Br 11.8% Stabilized PCE of 11.5% (stored in the dark with encapsulations). [88]
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