Research progress on large-area all-inorganic perovskite solar cells
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摘要: 近年,全无机钙钛矿太阳电池因其具有优良的光电性能及优异的热稳定性成为光伏领域的关注热点之一。该类电池现获得了21.15%的光电转换效率(PCE),并且还有望得到进一步地提高。然而,目前获得高效率全无机钙钛矿电池的有效面积都相对较小,多数处于0.1 cm2水平,大面积全无机钙钛矿太阳电池的PCE会因有效面积的增加而大幅降低。而大面积电池的制备对于全无机钙钛矿太阳电池的商业化应用极其重要。为了让全无机钙钛矿类材料在光伏领域上得到更好地应用,对全无机钙钛矿构建多组分复合材料结构及制备工艺调整是最简单而有效的方法。本文针对目前大面积全无机钙钛矿太阳电池进行系统综述,对较大面积的全无机钙钛矿太阳电池已取得的成果进行总结。针对目前大面积全无机钙钛矿太阳电池所处现状进行分析,并且对可制备大面积钙钛矿太阳电池的工艺及电池性能优化策略进行了系统性的归纳,最后对其领域未来发展趋势进行了展望。Abstract: In recent years, all-inorganic perovskite solar cells have become a hot topic in the photovoltaic field due to their excellent optoelectronic properties and outstanding thermal stability. This type of cell has achieved a photovoltaic conversion efficiency (PCE) of 21.15%, and further improvements are expected. However, the effective area of currently efficient all-inorganic perovskite cells is relatively small, mostly around 0.1 cm2, and the PCE of large-area all-inorganic perovskite solar cells will decrease significantly with an increase in effective area. The preparation of large-area cells is crucial for the commercial application of all-inorganic perovskite solar cells. In order to make all-inorganic perovskite materials better apply in the photovoltaic field, it is the simplest and most effective method to construct a multi-component composite structure and adjust the preparation process of all-inorganic perovskite. This article provides a systematic review of the progress in large-area all-inorganic perovskite solar cells, summarizing the achievements of all-inorganic perovskite solar cells with larger area. An analysis of the current status of large-area all-inorganic perovskite solar cells is also presented, and systematic summaries are given for the process of preparing large-area perovskite solar cells and strategies for optimizing cell performance. Finally, the future development trends in this field are discussed.
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图 3 PbBr2薄膜和CsPbBr3薄膜的水基喷雾辅助生长策略和形貌特征的说明:(a) 通过水基喷雾辅助生长策略制备CsPbBr3薄膜;(b) PbBr2薄膜的SEM图像;((c)~(g)) 分别使用30 μL、60 μL、90 μL、120 μL和150 μL的CsBr/H2O 制备出CsPbBr3薄膜的SEM图像[80]
Figure 3. Water-based spray-assisted growth strategy and morphology of PbBr2 and CsPbBr3 thin films: (a) CsPbBr3 films prepared by a water-based spray-assisted growth strategy; (b) SEM image of PbBr2 film; ((c)-(g)) SEM images of CsPbBr3 thin films prepared by using 30 μL, 60 μL, 90 μL, 120 μL and 150 μL CsBr/H2O, respectively[80]
DMF—N, N-dimethylformamide
图 5 旋涂的SnOx膜(a)、溅射的SnOx膜(b)和溅射的Ga(5%)-SnOx膜(c)的顶视图SEM图像;沉积在旋涂的SnOx膜(d)、溅射的SnOx膜(e)和溅射的Ga(5%)-SnOx膜(f)上的CsPbBr3膜的顶视图SEM图像[85]
Figure 5. Top view SEM images of spin-coated SnOx film (a), sputtered SnOx film (b) and sputtered Ga(5%)-SnOx film (c); Top-view SEM images of CsPbBr3 films deposited on spin-coated SnOx film (d), sputtered SnOx film (e) and sputtered Ga(5%)-SnOx film (f)[85]
图 6 ((a), (d), (g)) 沉积态CsPbBr3薄膜表面和横截面SEM图像;((b), (e), (h)) 400℃的CsPbBr3薄膜表面和横截面SEM图像;((c), (f), (i)) 500℃退火的CsPbBr3薄膜表面和横截面SEM图像;(j) 双源真空蒸发沉积制备CsPbBr3全无机钙钛矿薄膜;(k) CsPbBr3全无机钙钛矿太阳电池的光电转换效率 (PCE)和面积[16]
Figure 6. ((a), (d), (g)) SEM images of the surface and cross-section of the deposited CsPbBr3 film; ((b), (e), (h)) SEM images of the surface and cross-section of the CsPbBr3 film at 400℃; ((c), (f), (i)) SEM images of the surface and cross-section of the CsPbBr3 film annealed at 500℃; (j) CsPbBr3 all-inorganic perovskite film prepared by dual-source vacuum evaporation deposition; (k) Photo-voltaic conversion efficiency (PCE) and area of CsPbBr3 all-inorganic perovskite solar cell[16]
图 7 (a) 顺序蒸发技术制备CsPbBr3钙钛矿的示意图;(b) 制备的不同前体厚度比 (r)的溴化铯铅薄膜的数码相机图像;(c) 不同r值下CsPb2Br5相到CsPbBr3相再到Cs4PbBr6相的晶体结构转变示意图(底部的箭头表示相变过程)[101]
Figure 7. (a) Schematic diagram of CsPbBr3 perovskite prepared by sequential evaporation technique; (b) Digital camera images of cesium lead bromide films with different precursor thickness ratios (r) were prepared; (c) Crystal structure transition diagram of CsPb2Br5 phase to CsPbBr3 phase to Cs4PbBr6 phase under different r values (Arrow at the bottom represents the phase transition process)[101]
图 8 (a) 蒸发室示意图;(b) 蒸发的CsPbI3薄膜的照片(观察到两个明显不同的区域:黄色、棕色);(c) XRF测量的[Cs]/[Pb]原子比是垂直于相界测量的位置的函数(背景中的黄色和棕色相标有颜色)[103]
Figure 8. (a) Schematic diagram of the evaporation chamber; (b) Photo of the evaporated CsPbI3 film (Two distinct regions can be observed: One yellow, one brown); (c) [Cs]/[Pb] atomic ratio measured by XRF is a function of the position perpendicular to the phase boundary measurement (Yellow and brown phases in the background are colored)[103]
图 9 (a) CsPbBr3薄膜单源真空热蒸发沉积装置示意图;(b) 典型沉积CsPbBr3薄膜样品的照片;(c)从350到850 nm不同厚度沉积的CsPbBr3薄膜的表面SEM图像[104]
Figure 9. (a) Schematic diagram of a single-source vacuum thermal evaporation deposition device for CsPbBr3 thin film; (b) Photos of typical deposited CsPbBr3 thin film samples; (c) SEM images of the surface of CsPbBr3 films deposited at different thicknesses from 350 to 850 nm[104]
表 1 小面积(<0.1 cm2)全无机钙钛矿太阳电池的转换效率及其参数
Table 1. Conversion efficiency and parameters of small area (< 0.1 cm2) all-inorganic perovskite solar cells
Year Chart cell type Efficiency/% Area/cm2 Ref. 2017 ITO/Ca/C60/CsPbI3/TAPC/TAPC:MoO3/Ag 9.40 0.051 [14] 2017 FTO/TiO2/AX-CsPbI3 QDs/Spiro-OMeTAD/MoOx/Al 13.34 0.058 [15] 2018 FTO/c-TiO2/CsPbBr3/Spiro-OMeTAD/Au 6.95 0.09 [16] 2018 FTO/TiO2/CsPbBrI2/P3 HT/Au 12.02 0.05 [17] 2018 FTO/TiO2/CsPbBrI2 with DMSO-adducts/Spiro-OMeTAD/Au 14.78 0.09 [18] 2018 FTO/c-TiO2/m-TiO2/
PVP-CsPbI3/Spiro-OMeTAD/Au10.74 0.09 [19] 2019 FTO/TiO2(CsBr)/CsPbBr2I/Carbon 10.71 0.09 [20] 2019 FTO/c-TiO2/m-TiO2/
2%Ca2+-doped γ-CsPbI3/Spiro-OMeTAD/Au9.20 0.09 [21] 2019 FTO/c-TiO2/
CEG1.0MAICsPbI3/P3 HT/Au14.10 0.0919 [22] 2019 FTO/TiO2/Pb(SCN)2:2%-CsPbI3/PTAA/Au 17.04 0.09 [23] 2020 FTO/TiO2/BAI:CsPbBr2I/
Spiro-OMeTAD/Au10.78 0.09 [24] 2020 FTO/c-TiO2/mp-TiO2/2-ThPy-CsPbI2Br/Spiro-OMeTAD/Ag 12.69 0.09 [25] 2020 FTO/TiO2/NSs/CsPbBrI2/NSs/
Spiro-OMeTAD/Au16.65 0.09 [26] 2020 FTO/c-TiO2/mp-TiO2/
Cs0.99Rb0.01PbI2Br/P3 HT/Au17.16 0.09 [27] 2021 FTO/bl-TiO2/
Graded CsPbBrxI3−x/PTAA/Au16.81 0.096 [28] 2021 FTO/c-TiO2/SDMS-CsPbI3/
Spiro-OMeTAD/Au20.37 0.094 [29] 2022 FTO/TiO2/CsPbI2Br/BN-DHI/Carbon 14.14 0.075 [30] 2022 ITO/SnO2/CsPbI2Br/PCDA/Au 11.01 0.055 [31] 2022 ITO/NiMgLiO/CsPbI2Br/E-CdS/Au 15.04 0.09 [32] 2022 FTO/TiO2/Gly-X:CsPbI2Br/Spiro-OMeTAD/Au 17.26 0.09 [33] 2023 ITO/NiOx/CsPbI2.85Br0.15/PCBM/BCP/Ag 20.38 0.08875 [34] 2023 FTO/TiO2/γ-CsPbI3/Spiro-OMeTAD/Au 21.15 0.09 [8] Notes: ITO—Indium tin oxide; TAPC—4, 4′-cyclohexylidenebis[N, N-bis(4-methylphenyl)benzenamine]; FTO—Fluorine-doped tin oxide; AX—A-site cation halide salt; QDs—Quantum dot films; Spiro-OMeTAD—2, 2', 7, 7'-tetrakis[N, N-di(4-methoxyphenyl)amino]-9, 9'-spirobifluorene; c-TiO2—Crystalline titanium dioxide; P3 HT—Poly (3-hexylthiophene-2,5-diyl); DMSO—Dimethylsulfoxide; m-TiO2—Mesoporous titanium dioxide; PVP—Poly-vinylpyrrolidone; CEG—Cation exchange growth; MAI—Methylammonium iodide; PTAA—Poly[bis(4-phenyl) (2, 4, 6-trimethylphenyl)amine; BAI—n-butylammonium iodide; 2-ThPy—2-(2′-thienyl)pyridine; NSs—Nanosheets; mp-TiO2—Mesoporous titanium dioxide; bl-TiO2—Black titanium dioxide; SDMS—Stabilized-doped multi-cation single-crystalline; BN-DHI—2-bromonaphthalene-dynamic healing interface; PCDA—Poly[(9-alkyl-9H-carbazole-2, 7-diyl)-co-(2, 4-dimethylaniline-N, N-diyl)]; E-CdS—Electrodeposited cadmium sulfide; Gly-X—Glycine halides; PCBM—Phenyl-C61-butyric acid methyl ester; BCP—Bathocuproine. 表 2 大面积(≥0.1 cm2)全无机钙钛矿太阳电池的转换效率及参数
Table 2. Conversion efficiency and parameters of large area (≥ 0.1 cm2) all-inorganic perovskite solar cells
Year Chart cell type Efficiency/% Area/cm2 Ref. 2016 FTO/c-TiO2/CsPbBr2I/Au 4.70 0.159 [35] 2017 FTO/c-TiO2/CsPbBrI2/P3 HT/Au 6.70 0.159 [36] 2017 FTO/c-TiO2/CsPbBrI2/P3 HT/Au 5.50 1.20 [36] 2017 FTO/c-TiO2/mp-TiO2/
CsPb0.98Sr0.02BrI2/P3 HT/Au10.80 0.159 [37] 2017 FTO/c-TiO2/
Cs0.925K0.075PbBrI2/Spiro-OMeTAD/Au10.00 0.15 [38] 2017 FTO/c-TiO2/
CsPbI3·xEDAPbI4/Spiro-OMeTAD/Ag11.80 0.12 [39] 2018 FTO/c-TiO2/CsPbBr3/Spiro-OMeTAD/Au 5.37 1.00 [16] 2018 FTO/c-TiO2/m-TiO2/
Cs0.91Rb0.09PbBr3/Carbon7.07 >1.00 [40] 2017 ITO/SnO2/C60/
CsPb0.75Sn0.25Br2I/Spiro-OMeTAD/Au11.53 0.10 [41] 2018 FTO/TiO2/CsPbBrI2 with
DMSO-adducts/Spiro-OMeTAD/Au12.80 0.49 [18] 2018 FTO/TiO2/CsPbBrI2 with
DMSO-adducts/Spiro-OMeTAD/Au11.61 1.00 [18] 2018 ITO/SnO2/PEA-CsPbI3/Spiro-OMeTAD/Au 12.41 81 [42] 2019 FTO/TiO2/SmBr3/CsPbBr2I/PTAA/Au 10.88 2.00 [43] 2019 FTO/bl-TiO2/Sn doped CsPbI3/CuSCN/Au 3.09 0.25 [44] 2020 ITO/SnO2/MgO/CsPbBr2I/
Spiro-OMeTAD/Ag11.04 0.11 [45] 2020 FTO/SnO2/PANI-CsPbBrI2/Carbon 13.52 0.10 [46] 2021 FTO/bl-TiO2/Graded CsPbBrxI3−x/PTAA/Au 13.82 112 [28] 2021 ITO/ZnO/SnO2/
PEACl-KBr-CsPbI2Br/
Spiro-OMeTAD/MoO3/Ag16.90 0.12 [47] 2022 FTO/TiO2/GdCl3:CsPbI2Br/
Spiro-OMeTAD/Au16.24 0.1 [48] 2022 FTO/TiO2/CsPbI3/Spiro-MeOTAD/Au 20.06 1.0 [49] 2023 FTO/TiO2/CsPbI3−xBrx/Spiro-OMeTAD/Au 17.21 1.0 [50] 2022 ITO/PTAA/CsPbI3/OMXene-CsPbI3 composite/CPTA/BCP/Ag 14.64 25 [51] 2023 FTO/TiO2/CsPbI3/PCBM/Carbon 16.33 25 [52] 2023 FTO/TiO2/CsPbI3/Spiro-OMeTAD/Au 16.60 12 [53] Notes: CsPbI3·xEDAPbI4—Cesium lead iodide and ethylenediammonium lead iodide perovskite; PEA—Phenylethylammonium; PANI—Polymer additive polyaniline; PEACl—Phenylethylammonium chloride; OMXene—Oxygen-mediated MXene. 表 3 大面积全无机钙钛矿薄膜制备方法
Table 3. Preparation method of large area all-inorganic perovskite film
Preparation method Advantage Disadvantage Ref. Preparation method Advantage Disadvantage Ref. Spin coating method The film is relatively uniform and the thickness of the film is controllable Low crystal structure and purity [58]
Chemical vapor deposition methodHigh purity and good uniformity of thin films Complex equipment, high cost, and high requirements for reaction conditions [63] Spray coating method Suitable for complex substrate materials and non flat surfaces Easily prone to defects and requires high solvent selectivity [59] Sequential evaporation method Good precision control, film uniformity, and repeatability High equipment requirements and interface defects [64] Slot-die coating method High throughput and
low costLiquidity limitations may limit the thickness and uniformity of the film [60] Co-evaporation method Good uniformity and high repeatability of the film High requirements for parameters such as evaporation rate and distance between evaporation sources [65] Blade-coating method Simple, low-cost,
suitable for large
area substratesLimitations on film thickness and uniformity [58] Flash evaporation method Fast, simple, and
efficientHigh selectivity for solvents [66] Ink-jet
printing methodHigh precision and flexibility Ink jet head blockage and droplet size control [61] Vacuum thermal evaporation method The process of paper
cup thin film does not require solvents, and
high purity thin film depositionVacuum equipment is relatively complex and has a high investment cost [67] Vacuum
flash-assisted solution methodHigh speed, simple, suitable for various materials and
substratesComplex equipment and high cost [62] Multi-flow air knife method High speed coating,
good uniformity,
coating saving, and
wide applicabilityComplex equipment, difficult process control, not suitable for high viscosity coatings [68] -
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