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Progress in Chemistry 2020, Vol. 32 Issue (10): 1608-1632 DOI: 10.7536/PC200313 Previous Articles   

All-Inorganic Perovskite Solar Cells: Status and Future

Xiaohui Ma1, Liqun Yang1, Shijian Zheng1, Qilin Dai2, Cong Chen1,3,**(), Hongwei Song3,**()   

  1. 1. School of Material Science and Engineering, Hebei University of Technology, Tianjin 300130, China
    2. Department of Chemistry, Physics, and Atmospheric Sciences, Jackson State University, Jackson, Mississippi 39217, U.S.A.
    3. State Key Laboratory of Integrated Optoelectronics, College of Electronic Science and Engineering, Jilin University, Changchun 130012, China
  • Received: Revised: Online: Published:
  • Contact: Cong Chen, Hongwei Song
  • About author:
    **e-mail:(Cong Chen)
    (Hongwei Song)
  • Supported by:
    National Natural Science Foundation of China(51771201); National Key Research and Development Plan of China(2016YFC0207101)
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In recent years, organic-inorganic hybrid perovskite materials based on the ABX3 structure have attracted worldwide attention due to their excellent optoelectronic properties and cheap manufacturing costs. However, the organic components in the system are elementary to be resolved under the influence of light, heat, humidity, and other external conditions, which greatly limits the industrialization of the PSCs(Perovskite solar cells). All-inorganic perovskite materials prepared by using pure inorganic cations to replace the A-site organic cations in ABX3 structure have been developed rapidly due to their excellent thermal stability and environmental stability. At present, the efficiency of all-inorganic perovskite solar cells(I-PSCs) has exceeded 19% with broad application prospects. The research progress of inorganic perovskite materials and the different types of inorganic perovskite materials are reviewed. Meanwhile, the ways to improve the stability of devices from the aspects of films forming process, doping engineering, post-processing engineering, etc. are summarized Finally, we introduced the large-area preparation and flexible application of I-PSCs, reveals the challenges faced by I-PSCs and summarizes the prospect of the field.

Contents

1 Introduction

2 Basic of I-PSCs

2.1 Crystal structure of inorganic perovskite

2.2 Working principle of I-PSCs

2.3 Device structure of I-PSCs

3 Preparation process of inorganic perovskite

3.1 Solution processing technology

3.2 Vacuum preparation technology

3.3 Other preparation methods

4 Inorganic Pb-based perovskite and devices

4.1 CsPbI3

4.2 CsPbBr3

4.3 CsPbI3-xBrx

4.4 Cs1+xPbI3+x

5 Inorganic Sn/Ge-based perovskite and devices

5.1 CsSnI3

5.2 CsSnBr3

5.3 CsSnI3-xBrx

5.4 CsGeI3

6 Perovskite derivatives and devices

7 Functional application of inorganic perovskite

8 Stability of inorganic perovskite

8.1 Phase stability

8.2 Light and thermal stability

9 Large-area preparation and flexible application

10 Conclusion and outlook

Key words: all-inorganic, perovskite solar cells, doping, thermal stability, phase stability
Fig.1 The development of CsPbX3 PSCs
Fig.2 (a) Crystal structure of inorganic perovskite[38]; (b) energy level diagram of I-PSCs[39]; (c) device structure of I-PSCs[40]; (d) one-step solution method[39]; (e) two-step solution method[39]; (f) vacuum processing technique[39]; (g) vapor assisted/spray assisted solution approach[41]
Fig.3 (a) Crystal structure of CsPbI3[43]; (b) Schematic diagram of zwitterionic stabilized α-CsPbI3[46]; (c) Schematic diagram of CsPbI3·xDETAI3 PSCs[47]; (d) J-V curve of CsPbI3·xDETAI3 PSCs[47]; (e) Stability test curves of CsPbI3·0.05DETAI3 PSCs in dark dry box[47]
Fig.4 (a) Stabilization of α-CsPbI3 by adding HI or Bi3+ in the precursor solution[49]; (b) Schematic diagram of CsPbI3 film surface passivation principle[50]; (c) Cross section SEM image of PTABr-CsPbI3 PSCs[50]; (d) CsPbI3 crack filling interface engineering schematic[53]; (e) Forward and reverse scanning J-V curve and (f) stability test curve of CHI-CsPbI3 PSCs[53]
Fig.5 (a) Schematic of the film deposition process and AX salt posttreatmnet[55]; (b) Schematic drawing of the charge transport process and stabilization mechanism for the μGR/CsPbI3 film based PSCs[57]; (c) Photographs of CsPbI3 QD solutions with increasing Yb-doping concentrations and solutions under UV illumination[59]; (d) J-V curve and (e) stability test curve of 20% Yb-CsPbI3 quantum dots PSCs[59]
Fig.6 (a) J-V curves of different all-inorganic PSCs[62]; (b) SEM images of CsPbIBr2 film surface treated with guanidinium iodide at different concentrations[67]; (c) J-V curve and (d) stability test curve of CsPbIBr2 PSCs[67]; (e) The scheme of device architecture of I-PSCs, LiF was used to modify the SnO2 surface[75]; (f) Energy band alignment for each layer in CsPbI3-xBrx PSCs[75]
Table 1 Structure and performance of CsPbX3 (X=I, Br or I and Br) PSCs
Device configuration Voc
(V)		 Jsc
(mA·cm-2)		 FF
(%)		 PCE
(%)		 Year ref
FTO/TiO2/CsPbI3/Spiro-OMeTAD/Au — — — 2.90 2015 19
FTO/TiO2/CsPbI3/Spiro-OMeTAD/Ag 0.66 11.92 52.47 4.13 2016 78
FTO/TiO2/CsPbI3 QDs/Spiro-OMeTAD/MoOx/Al 1.23 13.47 65.00 10.77 2016 23
FTO/TiO2/CsPbI3 QDs/Spiro-OMeTAD/MoOx/Al 1.16 15.24 76.63 13.43 2017 55
FTO/TiO2/CsPbI3·0.025EDAPbI4/Spiro-OMeTAD/Ag 1.15 14.53 71.00 11.86 2017 79
FTO/c-TiO2/CsPb0.96Bi0.04I3/CuI/Au 0.97 18.76 72.59 13.21 2017 49
FTO/c-TiO2/CsPbI3·xDETAI3/P3HT/Au 1.06 12.20 61.00 7.89 2018 47
FTO/TiO2/CsPbI3/PTAA/Au 1.05 18.95 74.90 15.07 2018 44
FTO/TiO2/PTABr-CsPbI3/Spiro-OMeTAD/Ag 1.10 19.15 80.60 17.06 2018 50
FTO/TiO2/γ-CsPbI3/P3HT/Au 1.04 16.53 65.70 11.30 2018 51
N-GQD/FTO/TiO2/γ-CsPbI3/PTAA/Au 1.10 19.15 75.60 16.02 2019 80
FTO/c-TiO2/β-CsPbI3/Spiro-OMeTAD/Ag 1.11 20.23 82.00 18.40 2019 53
FTO/m-TiO2/CsPbBr3/PTAA/Au 1.28 6.24 74.00 5.95 2015 31
FTO/TiO2/CsPbBr3/C 1.24 7.40 73.00 6.70 2016 81
FTO/c-TiO2/m-TiO2/CsPb0.97Sm0.03Br3/C 1.59 7.48 85.10 10.14 2018 61
FTO/c-TiO2/m-TiO2/CsPb0.97Tb0.03Br3/SnS:ZnS/NiOx/C 1.57 8.21 79.60 10.26 2018 62
FTO/TiO2/PTI-CsPbBr3/Spiro-OMeTAD/Ag 1.49 9.78 74.47 10.91 2019 60
FTO/m-TiO2/CsPbIBr2/Spiro-OMeTAD/Al 1.12 7.80 72.00 6.30 2016 29
ITO/PEDOT:PSS/CsPbI2Br/PCBM/BCP/Al — — — 6.80 2016 63
FTO/c-TiO2/Cs0.925K0.075PbI2Br/Spiro-OMeTAD/Au 1.18 11.60 73.00 10.00 2017 68
FTO/mp-TiO2/CsPb0.98Sr0.02I2Br/P3HT/Au 1.04 15.30 69.90 11.30 2017 69
FTO/m-TiO2/CsPb0.9Sn0.1IBr2/C 1.26 14.30 63.00 11.33 2017 70
ITO/Ca/C60/CsPbI2Br/TAPC/TAPC:MoO3/Ag 1.17 15.50 68.00 11.80 2017 82
ITO/TiO2/CsPbI2Br/P3HT/Au 1.30 13.13 70.40 12.02 2018 74
ITO/SnO2/CsPbI2Br/Spiro-OMeTAD/Ag 1.06 15.99 77.12 13.09 2018 66
FTO/TiO2/CsPbBrI2/CsPbI2Br QDs/PTAA/Au 1.22 15.10 80.30 14.81 2018 65
FTO/NiOx/InCl3:CsPbI2Br/ZnO@C60/Ag 1.14 15.70 77.00 13.74 2018 71
ITO/SnO2/ZnO/CsPbI2Br/Spiro-OMeTAD/MoO3/Ag 1.23 15.00 78.80 14.60 2018 73
ITO/SnO2/CsPbI2Br/PTAA/MoO3/Al 1.19 15.66 74.10 13.80 2019 83
ITO/TiO2/CsPbI2Br/PTAA/Au 1.31 14.55 78.58 14.86 2019 84
ITO/SnO2/LiF/CsPbI3-xBrx/Spiro-OMeTAD/Au 1.22 18.20 80.97 18.64 2019 75
Fig.7 (a) Crystal structure of CsSnI3 (The red balls represent "I", the yellow balls represent "Sn", and the blue balls represent "Cs")[87]; (b) Cross sectional SEM image of CsSnI3 PSCs[91]; (c) J-V curves of photovoltaic devices fabricated with different amounts of SnF2 addition[91]; (d) Schematic diagram of CsSnI3 PSCs[92]; (e) J-V curves of CsSnI3 PSCs after annealing at different temperatures[92]; (f) J-V curve of CsSnI3 PSCs with optimum performance[92]
Fig.8 (a) Energy band positions of CsSnBr3 under different conditions[99]; (b) Tauc plots of the CsSnI3-xBrx with different x values[101]; (c) Relation of the band gap of CsSnI3-xBrx with x values[101]; (d) Energy level diagram of each material and charge transportation within a PSC[103]; (e) The crystal structure of CeGeI3 (R3m on the left, Pmmm on the right)[108]; (f) TEM images of CsGeI3 nanocrystals under different exposure times[110]
Table 2 Structure and performance of CsSnX3 (X=I, Br or I and Br) PSCs
Device configuration Voc
(V)		 Jsc
(mA·cm-2)		 FF
(%)		 PCE
(%)		 Year Ref
ITO/CsSnI3/Au/Ti 0.42 4.80 22.00 0.88 2012 10
FTO/c-TiO2/m-TiO2/20 mol%SnF2-CsSnI3/m-MTDATA/Au 0.24 22.70 37.00 2.02 2014
91
FTO/c-TiO2/m-TiO2/20 mol%SnF2-CsSnI3/Spiro-OMeTAD/Au 0.20 27.67 29.00 1.66 2015
101
ITO/NiOx/CsSnI3/PCBM/Al 0.52 10.21 62.50 3.31 2016
92
ITO/10 mol%SnCl2-CsSnI3/PCBM/BCP/Al 0.51 10.35 69.00 3.56 2016
93
FTO/bl-TiO2/10 mol%SnBr2-CsSnI3/PTAA/Au 0.44 18.50 52.90 4.30 2018
111
FTO/bl-TiO2/10 mol%SnCl2-CsSnI3/PTAA/Au 0.43 17.40 52.30 3.90 2018
111
FTO/bl-TiO2/10 mol%SnI2-CsSnI3/PTAA/Au 0.41 18.00 46.30 3.40 2018
111
FTO/PCBM/CsSn0.5Ge0.5I3/Native oxide/Spiro-OMeTAD/Au 0.63 18.61 60.60 7.11 2019
94
ITO/PEDOT/CsSnI3/PCBM/Ag — — — 5.03 2019
95
FTO/c-TiO2/m-TiO2/20 mol%SnF2-CsSnBr3/Spiro-OMeTAD/Au 0.41 3.99 58.00 0.95 2015
101
FTO/m-TiO2/CsSnBr3/Spiro-OMeTAD/Au 0.42 9.10 57.00 2.17 2016
98
ITO/MoO3/2.5 mol%SnF2-CsSnBr3/C60/BCP/Ag 0.40 2.40 55.00 0.55 2016
97
FTO/c-TiO2/m-TiO2/20 mol%SnF2-CsSnBr3/PTAA/Au 0.37 13.96 59.36 3.04 2017
100
FTO/c-TiO2/m-TiO2/20 mol%SnF2-CsSnI2.9Br0.1/Spiro-OMeTAD/Au 0.22 24.16 33.00 1.76 2015
101
FTO/c-TiO2/m-TiO2/20 mol%SnF2-CsSnI2Br/Spiro-OMeTAD/Au 0.29 15.06 38.00 1.67 2015
101
FTO/c-TiO2/m-TiO2/20 mol%SnF2-CsSnIBr2/Spiro-OMeTAD/Au 0.31 11.57 43.00 1.56 2015
101
FTO/c-TiO2/m-TiO2/m-Al2O3/60 mol%SnF2+HPA-CsSnIBr2/C 0.31 17.40 57.00 3.20 2016
102
Fig.9 (a) XRD patterns of Cs2SnI6 powder after being left in air for different times[117]; (b) J-V curves of Cs2SnI6-xBrx PSCs, inset shows IPCE values for Cs2SnI6 (black) and Cs2SnBr2I4 (green)[112]; (c) SEM images of Cs2SnI6 powder synthesized with different proportions of precursors in different solvents, CsI∶SnI2 is 1∶1 (two pictures above), CsI∶SnI4 is 3∶2 (two pictures below)[118]; (d) UV-vis absorption and PL spectra of Cs2AgBiBr6 film[122]; (e) J-V curves of Cs2AgBiBr6 PSCs prepared by solution method and vacuum deposition method[16]; (f) SEM images of (Cs1-xRbx)2AgB6[125]
Table 3 Structure and performance of Cs2AgBiBr6 PSCs
Device configuration Voc
(V)		 Jsc
(mA·cm-2)		 FF
(%)		 PCE
(%)		 Year ref
FTO/c-TiO2/m-TiO2/Cs2AgBiBr6/Spiro-OMeTAD/Au 0.98 3.93 63.00 2.43 2017 124
ITO/SnO2/Cs2AgBiBr6/P3HT/Au 1.04 1.78 78.00 1.44 2018 123
ITO/Cu-NiO/Cs2AgBiBr6/C60/BCP/Ag 1.01 3.19 69.20 2.23 2018 121
FTO/c-TiO2/m-TiO2/Cs2AgBiBr6/PTAA/Au 1.02 1.84 67.00 1.26 2018 126
FTO/c-TiO2/m-TiO2/Cs2AgBiBr6/Spiro-OMeTAD/Au 0.64 2.45 57.00 0.90 2018 126
FTO/c-TiO2/m-TiO2/Cs2AgBiBr6/PCPDTBT/Au 0.71 1.67 57.00 0.68 2018 126
ITO/SnO2/(Cs0.9Rb0.1)2AgBiBr6/Spiro-OMeTAD/Au 0.99 1.94 72.00 1.39 2019 125
FTO/TiO2/Cs2AgBiBr6/Spiro-OMeTAD/MoO3/Ag 1.01 3.82 65.00 2.51 2019 16
Fig.10 (a) Schematic diagram of PSCs structure modified by nanocrystals, where CsPbBr3 was introduced into the devices[129]; (b) J-V curve of CsPbBr3@SiO2 PSCs[129]; (c) Schematic architecture of the modi?ed PSCs[130]; (d) J-V curves and (e) the stability of PSCs with and without Al2O3 encapsulation layer[130]
Fig.11 (a) Schematic diagram of CsPbBrCl2 quantum dots film deposition principle[132]; (b) Schematic diagram of improving the performance of silicon-based solar cells with perovskite film[133]; (c) J-V curves of the devices with different amounts of Nb doping[148]; (d) EDX analysis revealing the evolution of the iodine-to-lead atomic ratio in the CsPbI3 films when exposed to light[161]; (e) Comparison of photochemical degradation of the hybrid MAPbBr3 and all-inorganic CsPbBr3 perovskite material[161]
Fig.12 (a) Schematic diagram of improving perovskite film properties by blade-coating method and the physical diagram of the large area CsPbI2Br film[164]; (b) J-V curves of the CsPbI2Br PSCs based on different effective areas[165]; (c) J-V characteristics evolution of the flexible device upon increasing bending cycles at a fixed bending radius of 10 mm[167]; (d) J-V curve of the ?exible GAI-DEE-CsPbIBr2 (20 mg/mL) PSC based on the PET substrate[67]; (e) PCEs and photographs of GAI-CsPbIBr2 (20 mg/mL) PSC based on the FTO substrate with different active areas[67]
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