Progress on Large-area Organic-inorganic Hybrid Perovskite Films and Its Photovoltaic Application

doi:10.15541/jim20230448

Abstract

Abstract:

Recently, organic-inorganic hybrid perovskite solar cells have demonstrated a broad commercial prospect due to their high photoelectric conversion efficiency (PCE) and low fabricating costs. During the past decades, the highest reported PCE of small-area (<1 cm²) perovskite solar cells (PSCs) rose to 26.10%, and those of large-area (1-10 cm²), mini-module level (10-800 cm²) and module level (>800 cm²) PSCs increased to 24.35%, 22.40% and 18.60%, respectively. The performance of PSCs decreases dramatically with the area increasing due to limitation of the deposition method and the poor quality of large-area perovskite films. Spin-coating method is not suitable for actual industrial production, while the scalable deposition methods including blade-coating and slot-die coating still face the difficulty of precisely controlling nucleation and crystallization of the perovskite films with large area. This review summarized preparation methods of large-area perovskite films, and discussed the film-forming mechanism and strategies for high-quality perovskite films. Finally, relevant outlooks on technologies and applications for large-area PSCs with high performances and stabilities were analyzed. This review is expected to provide insights on the research of large-area PSCs with high performance.

Key words: perovskite film, perovskite solar cell, large area, film-forming control, review

CLC Number:

TQ174

ZHANG Hui, XU Zhipeng, ZHU Congtan, GUO Xueyi, YANG Ying. Progress on Large-area Organic-inorganic Hybrid Perovskite Films and Its Photovoltaic Application[J]. Journal of Inorganic Materials, 2024, 39(5): 457-466.

Figures/Tables 6

Fig. 1 Scalable-deposition techniques of large-area PSCs (a) Blade-coating; (b) Slot-die coating; (c) Bar coating[21]; (d) Inkjet printing[22]; (e) Screen printing[23]; (f) Co-evaporation[24]; (g) Vacuum flash-assisted solution process (VASP)[26]

Table 1 Summary of large area (≥1 cm2) perovskite layer composition, deposition techniques and corresponding PSCs performance

Perovskite layer composition	Deposition technique	V_OC/V	J_SC/(mA·cm^-2)	FF/%	PCE/%	Area/cm²	Ref.
FA_0.88Cs_0.12PbI₃	One-step blade-coating	1.00	21.21	72	15.30	205	[3]
MAPbI₃	One-step blade-coating	1.08	23.17	68	17.06	1	[16]
FAPbI₃	Two-step blade-coating	6.71	3.47	71	16.54	25	[17]
FAPbI₃	Two-step blade-coating	6.65	3.72	75	18.65	25	[18]
(FACs)Pb(IBr)	Vacuum evaporation+blade-coating	1.20 4.72	24.42 5.59	82 76	24.03 20.02	1 16	[19]
FA_0.15MA_0.85PbI₃	Screen printing	1.10	23.93	69	18.12	1	[23]
MAPbI₃	Co-evaporation	6.71	3.68	73	18.13	21	[24]
FA_0.81MA_0.15PbI_2.51Br_0.45	Two-step spin-coating+VASP	1.14	23.19	76	20.38	1	[26]
FA_0.995MA_0.005Pb(I_0.995Br_0.005)₃	Vacuum evaporation+spin-coating	1.18	24.55	77	22.26	1	[30]

Fig. 2 Film-forming mechanism of perovskite layer (a) LaMer model for nucleation and growth of perovskite films[5]; (b) Relationship between volumetric and interfacial energy for the energy barrier to form a nucleus[28]; (c) Photographs and PCEs of PSCs from devices fabricated on test areas of the respective substrates (>100 cm2) (u0: speed of air knife)[29]; (d) J-V curves of perovskite crystal array (PCA) treated PSCs[30]

Fig. 3 Composition engineering of perovskite material ABX3 (a) Schematic diagram of crystal structure of perovskite[32]; (b) J-V curves of solar modules based on W/O and W/Cs perovskite films[34]; (c) X-ray diffraction patterns of CsxFA1-xPbI1.8Br1.2 perovskite films[35]; (d) Roles of cations in the realized degradation routes[36] (IC: instability index); (e) Fill factor limitation comprises nonradiative loss (blue area) and transport loss (pink area)[39]; (f) J-V curves of 1.03 cm2 PSCs and 10.93 cm2 mini-module level PSCs with insets showing their pictures[39]; (g) Scanning electron microscopy (SEM) images of FACs perovskite films with different compositions[40]; (h) J-V curves of FACs perovskite solar cells with different compositions before and after light soaking[40]; (i) Pb4f high-resolution X-ray photoelectron spectra of perovskite films using PbI2 precursor films with light irradiation for 0-8 h[43]

Fig. 4 Additive engineering of perovskite precursor ink (a) SEM images of vapor deposited PbI2 (V-PbI2) with solution processed PbI2 (S-PbI2) as the control films, or solution processed NH4Cl-PbI2 films, and their corresponding perovskite films[60]; (b) J-V curve and picture of a large-area PSC (1.01 cm2) based on NpMAI (NpMA: 1-naphthalenemethylammounium) treated films[61]; (c) Digital images of two pieces of representative crown-FACsPbI3 films (16 and 100 cm2 area) [63]; (d) J-V curves for the champion sulfolane treated PSCs with 0.09, 0.16, and 1 cm2 working areas[64]; (e) J-V curves of a larger device (1 cm2) with perfluorobenzene (HFB)[65]; (f) PCE distributions of 10 independent PSCs with (target) and without (control) modification[66]; (g) J-V curve and photograph of a 5 cm×5 cm BTAI-MAPbI3 based perovskite solar module (PSM)[67]

Table 2 Summary of large area (≥1 cm2) perovskite layer composition, factors influencing the crystallinity (solvent system and additive type) and performance of corresponding PSCs

Perovskite layer composition	Factor affecting perovskite crystallinity		V_OC/V	J_SC/(mA·cm^-2)	FF/%	PCE/%	Area/cm²	Ref.
FA_0.83Cs_0.17PbI₃	Solvent system	DMF/NMP	15.35	1.67	76	19.54	65	[45]
MA_0.6FA_0.4PbI₃		2-ME/DMSO/CBH	5.81 16.07	4.25 1.53	78 78	18.126 19.15	18 50	[46]
(FAPbI₃)_0.875(CsPbBr₃)_0.125		DMF/DMPU	6.69	3.70	72	17.71	10	[47]
(FAPbI₃)_0.95(CsPbBr₃)_0.05		DMF/DMPU	10.82	2.15	77	17.94	20	[48]
FA_0.83Cs_0.17PbI_2.83Br_0.17		DMF/NMP/DPSO	1.08	20.63	74	16.63	21	[49]
(FAPbI₃)_0.95(MAPbBr₃)_0.05		2-ME/DMI	15.46	1.71	76	20.15	81	[50]
(FAPbI₃)_0.95(MAPbBr₃)_0.05		2-ME/CHP	5.79 11.79	4.54 2.14	80 81	20.99 20.40	15 31	[51]
MAPbI₃		2-ME/DMSO	3.19	7.19	70	14.57	2	[52]
FAPbI₃		2-ME/ACN	8.36	3.06	67	17.10	13	[53]
MAPbI₃		2-ME/DMSO/ACN	18.90	1.17	76	16.90	64	[54]
FAPbI₃		DMF/DMSO/ACN	9.00	3.14	76	21.90	16	[55]
Cs_0.03(FA_0.97MA_0.03)_0.97Pb(I_0.97Br_0.03)₃		DMF/DMSO/EtOH	1.19 3.50	23.98 7.57	74 72	21.04 18.95	1 3	[57]
(FAMA)PbI₃	Type of additive	NH₄Cl^a	7.31	2.96	67	14.55	25	[60]
(FAMA)PbI₃		NpMAI^a	1.19	24.53	76	22.26	1	[61]
(FACs)PbI₃		Crown	5.63 14.29	4.17 1.67	71 58	16.69 13.84	16 100	[63]
MAPbI₃		Sulfolane	7.44	3.04	71	16.06	37	[64]
FAPbI₃		Hexaflorobenzene	1.21	25.2	80	25.12	1	[65]
FAPbI₃		NAMHI	6.61	3.85	79	20.10	10	[66]
MAPbI₃		BTAI	6.52	3.51	80	18.57	12	[67]
FA_0.9MA_0.03Cs_0.07Pb(I_0.92Br_0.08)₃		PMA-AA	11.54	2.37	80	21.95	14	[68]

References 68

[1]	NREL. Best research-cell efficiency chart [2023-12-13]. https://www.nrel.gov/pv/cell-efficiency.html.
[2]	GREEN M A, DUNLOP E D, YOSHITA M, et al. Solar cell efficiency tables (version 62). Prog. Photovoltaics, 2023, 31(7): 651.
[3]	BU T L, ONO L K, LI J, et al. Modulating crystal growth of formamidinium-caesium perovskites for over 200 cm² photovoltaic sub-modules. Nat. Energy, 2022, 7(6): 528.
[4]	LIN H, YANG M, RU X N, et al. Silicon heterojunction solar cells with up to 26.81% efficiency achieved by electrically optimized nanocrystalline-silicon hole contact layers. Nat. Energy, 2023, 8(8): 789.
[5]	LEE J, LEE D, JEONG D, et al. Control of crystal growth toward scalable fabrication of perovskite solar cells. Adv. Funct. Mater., 2019, 29(47): 1807047.
[6]	关英翔. 大面积钙钛矿型太阳能电池及组件制作工艺. 北京: 北京信息科技大学硕士学位论文, 2015.
[7]	RONG Y G, HOU X M, HU Y, et al. Synergy of ammonium chloride and moisture on perovskite crystallization for efficient printable mesoscopic solar cells. Nat. Commun., 2017, 8: 14555. DOI PMID
[8]	PARIDA B, SINGH A, SOOPY A K K, et al. Recent developments in upscalable printing techniques for perovskite solar cells. Adv. Sci., 2022, 9(14): 220308.
[9]	丁建宁. 新型薄膜太阳能电池. 北京: 化学工业出版社, 2018: 81-82.
[10]	ZHANG H, ZHAO C X, YAO J X, et al. Dopant-free NiO_x nanocrystals: a low-cost and stable hole transport material for commercializing perovskite optoelectronics. Angew. Chem. Int. Ed., 2023, 62(24): e202219307.
[11]	LIU C, YANG Y, CHEN H, et al. Bimolecularly passivated interface enables efficient and stable inverted perovskite solar cells. Science, 2023, 382(6672): 810. DOI PMID
[12]	WU X, GAO D P, SUN X L, et al. Backbone engineering enables highly efficient polymer holetransporting materials for inverted perovskite solar cells. Adv. Mater., 2022, 35(12): 2208431.
[13]	CHEN Y, LIN P, CAI B, et al. Research progress of inorganic hole transport materials in perovskite solar cells. J. Inorg. Mater., 2023, 38(9): 991.
[14]	ZHU C T, GAO J, CHEN T, et al. Intrinsic thermal stability of inverted perovskite solar cells based on electrochemical deposited PEDOT. J. Energy Chem., 2023, 83: 445. DOI
[15]	PARK B W, KWON H W, LEE Y H, et al. Stabilization of formamidinium lead triiodide α-phase with isopropylammonium chloride for perovskite solar cells. Nat. Energy, 2021, 6(8): 419.
[16]	LI J B, MUNIR R, FAN Y Y, et al. Phase transition control for high-performance blade-coated perovskite solar cells. Joule, 2(7): 1313.
[17]	ZHANG J W, BU T L, LI J, et al. Two-step sequential blade-coating of high quality perovskite layers for efficient solar cells and modules. J. Mater. Chem. A, 2020, 8(17): 8447.
[18]	WEN Y T, LI J, GAO X F, et al. Two-step sequential blade-coating large-area FA-based perovskite thin film via a controlled PbI₂ microstructure. Acta Phys.-Chim. Sin., 2023, 32(2): 2203048.
[19]	TAN L G, ZHOU J J, ZHAO X, et al. Combined vacuum evaporation and solution process for high-efficiency large‐area perovskite solar cells with exceptional reproducibility. Adv. Mater., 2023, 35(3): 2205027.
[20]	杨志春, 吴狄, 剡晓波, 等. 大面积钙钛矿薄膜制备技术的研究进展. 材料导报, 2021, 35(1): 1046.
[21]	LI D Y, ZHANG D Y, LIM K S, et al. A review on scaling up perovskite solar cells. Adv. Funct. Mater., 2021, 31(12): 2008621.
[22]	CHEN Y J, WU H J, MA J J, et al. Droplet manipulation and crystallization regulation in inkjet-printed perovskite film formation. CCS Chem., 2022, 4(5): 1465.
[23]	CHEN C S, CHEN J X, HAN H C, et al. Perovskite solar cells based on screen-printed thin films. Nature, 2022, 612(7939): 266.
[24]	LI J, WANG H, CHIN X Y, et al. Highly efficient thermally co-evaporated perovskite solar cells and mini-modules. Joule, 2020, 4(5): 1035.
[25]	LEYDEN M R, JIANG Y, QI Y B, et al. Chemical vapor deposition grown formamidinium perovskite solar modules with high steady state power and thermal stability. J. Mater. Chem. A, 2016, 4(34): 13125.
[26]	LI X, BI D Q, YI C Y, et al. A vacuum flash-assisted solution process for high-efficiency large-area perovskite solar cells. Science, 2016, 353(6294): 58. DOI PMID
[27]	SANCHEZ S, PFEIFER L, VACHOPOUOUS N, et al. Rapid hybrid perovskite film crystalization form solution. Chem. Sov. Rev., 2021, 50(12): 7108.
[28]	LIU C, CHENG Y B, GE Z Y. Understanding of perovskite crystal growth and film formation in scalable deposition processes. Chem. Sov. Rev., 2020, 49(6): 1653.
[29]	GEISTERT K, TERNES S, RITZER D B, et al. Controlling thin film morphology formation during gas quenching of slot-die coated perovskite solar modules. ACS Appl. Mater. Interfaces, 2023, 15(45): 52519.
[30]	SHEN Z C, HAN Q F, LUO X H, et al. Crystal-array-assisted growth of a perovskite absorption layer for efficient and stable solar cells. Energy Environ. Sci., 2022, 15(3): 1078.
[31]	DUNLAP-SHOHL W A, ZHOU Y Y, PADTURE N P, et al. Synthetic approaches for halide perovskite thin films. Chem. Rev., 2019, 119(5): 3193. DOI
[32]	ZHENG Z W, WANG S Y, HU Y, et al. Development of formamidinium lead iodide-based perovskite solar cells: efficiency and stability. Chem. Sci., 2022, 13(8): 2167.
[33]	MUSCARELLA L A, EHRLER B. The influence of strain on phase stability in mixed-halide perovskites. Joule, 2022, 6(9): 2016.
[34]	LIU X H, CHEN M, ZHANG Y, et al. High-efficiency perovskite photovoltaic modules achieved via cesium doping. Chem. Eng. J., 2022, 431(4): 133713.
[35]	XIAO K, LIN H Y, ZHANG M, et al. Scalable processing for realizing 21.7%-efficient all-perovskite tandem solar modules. Science, 2022, 376(6594): 762. DOI PMID
[36]	SUN S J, TIIHONEN A, OVIEDO F, et al. A data fusion approach to optimize compositional stability of halide perovskites. Matter, 2021, 4(4): 1305.
[37]	SALIBA M, MATSUI T, DOMANSKI K, et al. Incorporation of rubidium cations into perovskite solar cells improves photovoltaic performance. Science, 2016, 354(6309): 206. PMID
[38]	ZHAO Y, MA F, QU Z H, et al. Inactive (PbI₂)₂RbCl stabilizes perovskite films for efficient solar cells. Science, 2022, 377(6605): 531.
[39]	CHANG J H, FENG E M, LI H Y, et al. Crystallization and orientation modulation enable highly efficient doctor-bladed perovskite solar cells. Nano-Micro Letter, 2023, 15(issue): 164.
[40]	DENG Y H, XU S, CHEN S S, et al. Defect compensation in formamidinium-caesium perovskites for highly efficient solar mini- modules with improved photostability. Nat. Energy, 2021, 6(6): 633.
[41]	JACOBSSON T J, CORREA-BAEBA J P, NARAKI E H, et al. Unreacted PbI₂ as a double-edged sword for enhancing the performance of perovskite solar cells. J. Am. Chem. Soc., 2016, 138(32): 10331.
[42]	MACPHERSON S, DOHERTY T A S, WINCHESTAR A J, et al. Local nanoscale phase impurities are degradation sites in halide perovskite. Nature, 2022, 607(7918): 294.
[43]	LIANG J W, HU X Z, WANG C, et al. Origins and influences of metallic lead in perovskite solar cells. Joule, 6(4): 816.
[44]	CHAO L F, NIU T T, GAO W Y, et al. Solvent engineering of the precursor solution toward large-area production of perovskite solar cells. Adv. Mater., 2021, 33(14): 2005410.
[45]	BU T L, LI J, LI H Y, et al. Lead halide-templated crystallization of methylamine-free perovskite for efficient photovoltaic modules. Science, 2021, 372(6548): 1327. DOI PMID
[46]	CHEN S S, DAI X Z, XU S, et al. Stabilizing perovskite-substrate interfaces for high-performance perovskite modules. Science, 2021, 373(6557): 902. DOI PMID
[47]	LI H Y, BU T, LI J, et al. Ink engineering for blade coating FA-dominated perovskites in ambient air for efficient solar cells and modules. ACS Appl. Mater. Interfaces, 2021, 13(16): 18724.
[48]	LEE D K, LIM K S, LEE J W, et al. Scalable perovskite coating via anti-solvent-free Lewis acid-base adduct engineering for efficient perovskite solar modules. J. Mater. Chem. A, 2021, 9(5): 3018.
[49]	YANG Z C, ZHANG W J, WU S H, et al. Slot-die coating large-area formamidinium-cesium perovskite film for efficient and stable parallel solar module. Adv. Sci., 2021, 7(18): eabg3749.
[50]	CHUNG J, KIM S, LI Y, et al. Engineering perovskite precursor inks for scalable production of high-efficiency perovskite photovoltaic modules. Adv. Energy Mater., 2023, 13(22): 2300595.
[51]	YOO J W, JANG J H, KIM U, et al. Efficient perovskite solar mini-modules fabricated via bar-coating using 2-methoxyethanol- based formamidinium lead tri-iodide precursor solution. Joule, 2021, 5(9): 2420.
[52]	LI J Z, DAGAR J, SHARGAIEVA O, et al. 20.8% slot-die coated MAPbI₃ perovskite solar cells by optimal DMSO-content and age of 2-ME based precursor inks. Adv. Energy Mater., 2021, 11(10): 2003460.
[53]	LI J Z, DAGAR J, SHARGAIEVA O, et al. Ink design enabling slot-die coated perovskite solar cells with >22% power conversion efficiency, micro-modules, and 1 year of outdoor performance evaluation. Adv. Energy Mater., 2022, 13(33): 2203898.
[54]	DENG Y H, BRACKE C H V, DAI X Z, et al. Tailoring solvent coordination for high-speed, room-temperature blading of perovskite photovoltaic films. Sci. Adv., 2019, 5(12): eaax7537.
[55]	YUAN L H, CHEN X N, GUO X M, et al. Volatile perovskite precursor ink enables window printing of phase-pure FAPbI₃ perovskite solar cells and modules in ambient atmosphere. Angew. Chem. Int. Ed., 2024, 63(7): e202316954.
[56]	NOEL N K, HABISREYTINGER S N, WENGER B, et al. A low viscosity, low boiling point, clean solvent system for the rapid crystallisation of highly specular perovskite films. Energy Environ. Sci., 2016, 10(1): 145.
[57]	LIANG Q, LIU K, SUN M, et al. Manipulating crystallization kinetics in high-performance blade-coated perovskite solar cells via cosolvent-assisted phase transition. Adv. Mater., 2022, 34(16): 2200276.
[58]	ZHAI P, REN L X, LI S Q, et al. Light modulation strategy for highest-efficiency water-processed perovskite solar cells. Matter, 2022, 5(12): 4450.
[59]	WANG W, ZHOU J, TANG W. Passivation strategies of perovskite film defects for solar cells. J. Inorg. Mater., 2022, 37(2): 129. DOI
[60]	TONG G Q, SON D, ONO L K, et al. Scalable fabrication of >90 cm² perovskite solar modules with >1000 h operational stability based on the intermediate phase strategy. Adv. Energy Mater., 2021, 11(10): 2003712.
[61]	ZHOU T, XU Z Y, WANG R, et al. Crystal growth regulation of 2D/3D perovskite films for solar cells with both high efficiency and stability. Adv. Mater., 2022, 34(17): 2200705.
[62]	MING Y, HU Y, MEI A, et al. Application of lead acetate additive for printable perovskite solar cell. J. Inorg. Mater., 2022, 37(2): 197. DOI
[63]	CHEN R H, WU Y Z, WANG Y K, et al. Crown ether-assisted growth and scaling up of FACsPbI₃ films for efficient and stable perovskite solar modules. Adv. Funct. Mater., 2021, 31(11): 2008760.
[64]	HUANG H H, LIU Q H, TSAI H, et al. A simple one-step method with wide processing window for high-quality perovskite mini-module fabrication. Joule, 2021, 5(4): 958.
[65]	HUANG Z J, BAI Y, HUANG X D, et al. Anion-π interactions supress phase impurities in FAPbI₃ solar cells. Nature, 2023, 623(2023): 531.
[66]	MENG Y Y, WANG Y L, LIU C, et al. Epitaxial growth of α-FAPbI₃ at a well-matched heterointerface for efficient perovskite solar cells and solar modules. Adv. Mater., 2024, 36(6): 2309208.
[67]	MIAO Y, REN M, WANG H F, et al. Surface termination on unstable methylammonium-based perovskite using a steric barrier for improved perovskite solar cells. Angew. Chem. Int. Ed., 2023, 62(51): e202312726.
[68]	LIU D C, CHEN C, WANG X Z, et al. Enhanced quasi-Fermi level splitting of perovskite solar cells by universal dual-functional polymer. Adv. Mater., 2023, 36(13): 2310962.