Recent Progress on Boosting the Perovskite Film Quality of All-Inorganic Perovskite Solar Cells

Abstract

All-inorganic CsPbX₃ perovskite material not only has the benefits of advanced light absorption coefficient, long carrier lifetime, and simple preparation process of organic–inorganic perovskite materials but it also maintains excellent stability under the erosion of damp heat. Stability is the premise of its industrialization, so all-inorganic perovskite is undoubtedly a very competitive direction for the development of perovskite materials. However, there are still many defects in the all-inorganic perovskite thin films, and it is difficult to obtain high power conversion efficiency (PCE). This review systematically summarizes additive engineering, solvent engineering, and interface engineering methods to promote the thin film property for a high PCE in recent years.

1. Introduction

Perovskite materials have attracted widespread attention in recent years due to their high light absorption coefficient, long carrier lifetime, low cost, simple preparation process [1,2,3,4], and ability for large-scale preparation [5,6,7,8]. The organic–inorganic hybrid perovskite solar cells (PSCs) have rapidly increased their power conversion efficiency (PCE) from 9.7% to over 25.5% [9,10,11,12]. However, in organic–inorganic hybrid perovskite devices, their organic parts, such as MA⁺ (CH₃NH₃⁺), FA⁺ ((CH(NH)₂)₂⁺), are easily affected and decomposed by the external temperature, illumination, and humidity [1,13,14,15,16,17], which leads to a serious decline in the PCE and stability [2,18]. For example, Juarez-Perez et al. [19] reported the decomposition temperature of MA⁺ was 80 °C, which was in the operating temperature range of PSCs. In 2015, Eperon et al. [20] for the first time prepared the all-inorganic CsPbI₃ cell and the PCE was 2.9%. This historic breakthrough provided a new idea to develop the PSCs. Liu et al. [21] revealed the PSCs based on Cs-doped MAPbI₃ can work steadily at 85 °C for 1000 h. They have manufactured modules (6.5 cm × 7 cm) with an advanced PCE of 21.08%. Steele et al. [22] found black CsPbI₃ was stable even at a high temperature of 330 °C. All-inorganic perovskite also showed smaller exciton binding energy, higher defect tolerance, and better photoelectric property [23,24,25]. In particular, a CsPbI₃ battery with an appropriate forbidden bandwidth of ~1.73 eV for the roof of a battery with silicon or other narrow band gap formation series battery [26,27]. All-inorganic perovskite solar cells have aroused wide public concern, as the PCE went to 21.0% in just a few years [28,29,30,31,32,33]. Although all-inorganic PSCs exhibited many excellent properties, their long-term development also faces many challenges, such as poor phase stability, high-density defects, and lower PCE. The property of the all-inorganic perovskite film affects the capability of the solar cells directly [34,35]. This review summarizes the main methods to obtain high-property all-inorganic perovskite films, including additive engineering, solvent engineering, and interface engineering. Then, we prospected the research direction and development prospect of all-inorganic PSCs in the future.

2. Film Quality Improvement

2.1. Additive Engineering

ABX₃ (A = Cs⁺, B = Pb²⁺, X = I⁻, Br⁻, Cl⁻) is the general formula crystal structure for all-inorganic perovskite materials [1,14,36,37,38]. As shown in Figure 1, there are four common crystal structures: the cubic phase (α-, Pm3m), the tetragonal phase (β-, P4/mbm), the orthorhombic phase (γ-, Pbnm), and the non-perovskite phase (δ-, Pnma) [39,40]. α, β, and γ phases are perovskite phases, and have a photovoltaic effect. They are also called black phases. However, they are only stable at high temperatures. At room temperature, these black perovskite phases will naturally transform into the yellow non-perovskite phase, which will seriously affect the performance of the PSCs [5,41]. The perovskite crystal structure stability can be calculated by the tolerance factor t: t = (R_A + R_B)/$\sqrt{2}$(R_B + R_X), where R_A, R_B, and R_X refer to the ionic radii of A, B, and X site ions, separately. Under normal conditions, if the crystal wants to maintain stability, the tolerance factor t needs to be in the range of 0.9–1. If the t value is less than this range, the crystal symmetry will be reduced and the entire structure stability will be affected. If the t value is more than this range, the system will occur a certain phase transition [38,42,43,44]. Therefore, in the research of all-inorganic perovskites, there is a certain theoretical basis for the selection of ions.

The method of additive engineering is an easy way to raise the stability of CsPbX₃ perovskite solar cells. Based on the tolerance factor t, lesser X-site anions mean bigger t values. The Br⁻ (1.96 Å) and Cl⁻ (1.81 Å) both have a smaller radius than I⁻ (2.2 Å), so some groups have added them into CsPbI₃. The CsPbI₃ structural stability increased with the bigger t values [9,25,26,45,46,47,48,49,50,51]. The SCN⁻ ion, a kind of pseudohalide ion, has a smaller radius, which could also strengthen the crystallization behavior of the CsPbI₃ film, and promoted the PCE to 17.03% [52]. Wang et al. [53] resoundingly synthesized high-property CsPbBr₃ films by adding 1.5% of NH₄SCN into the precursor solution, which contained NH4⁺ and pseudohalide ion SCN^-.

The lesser B-site cations are also good for phase stability [54]. Sn²⁺ and Pb²⁺ are both from group IVA and have similar physicochemical properties. The smaller Sn²⁺ ionic radius means a bigger t value, giving higher phase stability. Thus, Sn²⁺ is the most hopeful candidate to replace Pb²⁺. Murugadoss et al. [55] used different concentrations of Sn²⁺ doping to synthesize highly stable black phase CsPbI₃ films, improving the PCE to 5.12%. The alkali metal ions from the group ⅡA, such as Ca²⁺ [56], Sr²⁺ [57], and Ba²⁺ [58,59], have the same valence state as Pb²⁺, which are also potential competitors. In addition, Mn²⁺ could improve the stability of CsPbI₃ perovskite effectively [60,61,62]. Xu et al. found the appropriate amount of Cd²⁺ (1.0% mol of Pb²⁺) could improve the crystallinity of CsPbIBr₂, reduce its trap density, and suppress its photo-generated carrier recombination [63]. The trivalent smaller cations could also replace the B-site. Typical trivalent ions are Bi³⁺ [64], Sb³⁺ [65], Yb³⁺ [66], Eu³⁺ [67], In³⁺ [18], Er³⁺ [68], and Gd³⁺ [69]. Faheem et al. [68] deposited a series of different concentrations of trivalent anion Er^3- into CsPbIBr₂ perovskite. They found CsI-(PbBr₂)_0.97 (ErCl₃)_0.03 was the optimal ratio. The PCE of this solar cell was increased by about 60% (7.28%). Pu et al. [69] used different molar ratios of gadolinium chloride (GdCl₃) to increase the tolerance coefficient of CsPbI₂Br. The results showed that the 0.4% GdCl₃-incorporated CsPbI₂Br film had the highest PCE of 16.24%.

Since Eperon et al. [20] first prepared stable cubic CsPbI₃ films at room temperature by adding HI into its precursor solution, HI became the most common additive in CsPbI₃ PSCs. Some groups [70,71] suggested that the precursor solution with HI was a polar solvent, which could cause the α-CsPbI₃ to convert into the γ-CsPbI₃. Yu et al. [72] used 35 μL HI and 10 μL H₂O as additives to prepare high-quality CsPbI₃ films by one-step spin coating at 100 °C. In addition, the perovskite films containing micro-water had a smoother surface with bigger grain sizes. The grain interface was repaired by dissolution and recrystallization to obtain a smooth film after removing the water. The fill factor (FF) was increased from 62% to around 69% and the PCE was improved from 10.34% to 11.42%. However, some researchers reported that the water in the HI acid may give a passive effect to form perovskite. They used DMF instead of water. Zhang et al. [73] first used HPbI₃ to synthesize black CsPbI₃ perovskite films at 150 °C. Then, many groups added HPbI₃ in the precursor to prepare stable CsPbI₃ films [23,47,52,74,75,76,77,78]. The PSCs with the HPbI₃-treated CsPbI₃ have a PCE of over 18 % [48,78]. Xi et al. [79] found that adding more HI could get a new compound of H₂PbI₄. H₂PbI₄ could also increase the phase stability.

However, the mechanism of improving CsPbI₃ stability by HPbI₃ treatment is controversial. Some groups [80,81,82] found that the really useful material is DMAPbI₃, which was produced by the acid hydrolysis of DMF. DMA⁺ has a bigger radius than Cs⁺. When DMA⁺ partially replaced Cs⁺, it is easy to form a stable black phase. Some groups [78,83,84] had different opinions. They reported that annealing could remove most of the organic matter (DMA⁺), so only CsPbI₃ was left. Some groups [29,85] even added DMAI into the CsPbI₃ precursor immediately and got the best PCE of 19.03% [29].

Adding precursor material itself into the perovskite is also a good choice. Xiang et al. [86] added extra CsI into the precursor solution to synthesize black CsPbI₃ films in an air atmosphere at 110 °C. Becker et al. [87] showed that more CsI in the precursor could directly obtain the γ-CsPbI₃ perovskite phase. Their CsI-rich device gave a PCE of 12.5%. Bai et al. [88] controlled the ratio of CsI and PbI₂ in the precursor precisely. The best PCE based on the obtained 0D Cs₄PbI₆ and γ-CsPbI₃ heterojunction was 16.39%. Fu et al. [89] introduced excess CsBr into the CsPbI₃ precursor to prepare a more stable CsPbI₃ phase at low temperatures.

Fu et al. [90] added 2-hydroxyethyl methacrylate (HEMA) into the perovskite precursor to simultaneously increase the crystallization and decrease the deficiencies. The performance was best when 3 mg/mL HEMA was added. Yoon et al. [91] controlled the crystal growth procedure by adding a methylammonium chloride SDMS solution in continuous drops. Then, they used octyl ammonium iodides to passivate the surface in ambient air. CsPbI₃ with a 45 mM MACl film was highly uniform and pinhole-minimized. Li et al. [92] introduced 16.90 mg·mL⁻¹ CsPbBr₃ quantum dots on the surface of the CsPbI₃ film to passivate the deficiencies and improve the PCE to 16%. Zhang et al. [93] used the Zn²⁺ ions from zinc oxalate to recover the vacancies of Pb and Sn; then, they obtained perfect CsPb_0.7Sn_0.3IBr₂ films with high crystallinity and lower defect density. Wang et al. [94] improved the properties of CsPbIBr₂ films by bringing in a 3% molar ratio of guanidinium thiocyanate (GuaSCN), which was beneficial to optimize the PCE and stability of the PSCs. The various inorganic PSC performances using additive engineering are summarized in Table 1. Additive engineering was helpful for PSC performances. In addition to choosing the radius of the ions to add, the amount of material to add was also precisely controlled, as too many additions could have negative effects. Further, uncontrollable ionic components also greatly reduced the repeatability of the preparation process.

2.2. Solvent Engineering

Solvent engineering is a valid strategy to enhance the properties of perovskite for excellent PSCs [95]. Snaith et al. [25] prepared high-property CsPbI₂Br film for the first time by precisely controlling the dissolvability of CsPbI₂Br in DMF. McGehee et al. [27] used DMSO as the solvent to get high-property CsPbI₂Br films. Some groups [57,96,97,98,99] used dimethyl sulfoxide (DMSO) and dimethyl formamide (DMF) as co-solvents to obtain a CsPbI₂Br film, which could promote the solubility of CsPbI₂Br. Luo et al. [100] first obtained stable CsPbI₃ in fully open-air conditions by treating it with hydroiodic acid (HI) and isopropanol (IPA). Meng et al. [101] dissolved CsBr with ethylene glycol monomethyl ether (EGME) and IPA to control the Ostwald ripening. They got high crystalline and favorable CsPbBr₃ films. The EGME/IPA bi-solvent treatment increased the PCE from 3.57% to 7.29%.

With the increase of people’s awareness of environmental protection, green solvents are becoming more and more popular. He et al. [102] proved that green antisolvent IPA and thiourea can optimize the quality of CsPbIBr₂ films. The carbon-based CsPbIBr₂ PSCs have a PCE of 6.79%, which was almost 30% higher than the untreated PSCs. Wang et al. [103] replaced the noxious methanol with the environmentally friendly bi-component solvent (water and ethylene glycol monomethyl ether) to prepare high-property CsPbBr₃ films. The CsPbBr₃ PSC showed an optimal PCE of 9.55% with remarkable humidity stability. The eco-friendly ethyl acetate (EA) is another kind of solvent used in solvent engineering. Dong et al. [104] showed that the green EA antisolvent can optimize the properties of the CsPbI₂Br films. The EA-engineered CsPbI₂Br helped the PCE reach 10.0%. Han et al. [105] showed that the green EA antisolvent was able to promote better growth of the CsPbI₃ films. Saparbaev et al. [106] used eco-friendly methylammonium acetate liquid to assemble CsPbI₃ PSCs with a PCE of 14.4%.

Regulating the preparation process with solvent engineering is also a valid method to optimize the quality of the all-inorganic perovskite films. Wang et al. [24] adopted a solvent-controlled growth method to obtain a stable α-CsPbI₃ film. The CsPbI₃ solar cells showed a 15.7% PCE. Teng et al. [107] reported that the decomposition rate of the CsPbBr₃ precursor in a CsBr and methanol solution was faster, and CsPbBr₃ films synthesized by the traditional two-step approach had low quality. Zai et al. [108] developed an easy low-temperature solution process to carefully regulate the CsPbI₂Br crystallization kinetics, which increased PCE to 14.31%. The thermal and light stability was also perfect. Liu et al. [109] and Gao et al. [110] both applied a multistep spin-coating method to obtain the brilliant property of CsPbBr₃ films, which could improve the uniformity of nucleation. Wang et al. [111] found alcohol could cause a quick crystallization process of the CsPbIBr₂ films, which was very beneficial for improving its crystallinity. The obtained PSCs showed a high PCE of 11.49%. Wang et al. [112] adopted EAH-S solvent to extract the ammonium halide (Figure 2). This new strategy could solve the phase instability problems of CsPbI₃. The carbon-based CsPbI₃ PSCs attained a PCE of 15.35%. Zhong et al. [113] regulated the crystalline quality of CsPbBr₃ films by adding 2-phenethylamine bromide (PEABr) to the PbBr₂ DMF solution. The PCE increased to 8.25%. The PSCs’ performances related to solvent engineering are summarized in Table 2.

2.3. Interface Engineering

Interface engineering is also commonly used to modulate the morphology of perovskite films, stabilize the perovskite phase, and enhance operational stability [114,115]. Choosing contact materials and surface modification of the chosen contact materials are the main focuses of interface engineering research. For example, new materials are used in the electron transport layer (ETL). Yan et al. [116] introduced the SnO₂/ZnO bilayer ETL to obtain regular crystal grains and full coverage CsPbI₂Br films. Yue et al. [117] used the ZnO-doped TiO₂ buffer layer to improve the PCE to 21.06%, and the V_oc and FF were 1.31 V and 74.1%. Yang et al. [118] explored a better wettability surface of the In₂S₃ ETL to increase the rate of CsPbIBr₂ nucleation. Zhu et al. [119] presented a TiO₂/SnO₂ ETL that could control the CsPbIBr₂ crystallization. Li et al. [120] adopted a strategy of interface engineering by depositing the CsPbI₂Br perovskite film on a ZnO/Mg_xZn_1-xO bilayer ETL, which could alleviate energy loss in the PSCs. The best PCE was 16.04%. Pan et al. [121] chose well-arranged TiO₂ nanopillar arrays (TiO₂ NaPAs) to boost the interface of CsPbI₂Br and ETL, which resulted in continuously dense CsPbI₂Br films, with few defects. Guo et al. [122] improved the perovskite quality by the passivation of SnO₂ ETL. It could enhance the carrier transport across the ETL/CsPbIBr₂ boundary surface, raise the charge reorganization resistance, and reduce the E_loss for the ultimate PSCs. Lu et al. [123] took TiCl₄ treatment to enhance the perovskite film property for better PSCs. The PCE of TiCl₄-TiO₂- and TiCl₄-ZnO-based PSCs increased to 16.5% and 17.0%, respectively. Wang et al. [124] adopted the amino group from polyethyleneimine ethoxylated (PEIE) to inactivate the defects of CsPbIBr₂ and increase the PCE from 8.7% to 11.2%. Wang et al. [125] modified the interface of TiO₂/perovskite with CsAc, which enhanced the CsPbI_2.25Br_0.75 film morphology, crystallinity, and electrochemical properties. The PSCs based on the CsAc-modified method showed an optimized PCE of 13.81%. Chai et al. [126] added CsPbBr₃ seeds into the TiO₂ ETL to regulate the CsPbI₃ crystal growth and promote the PCE (Figure 3). This new method provided a new idea for the commercial application of PSCs.

The boundary surface between the perovskite and the hole transport layer (HTL) or electrode (without HTL) is another target to optimize perovskite film properties. Liu et al. [127] used a subtle MoOx cushion coat to raise the carrier injection, and reduce the trap state and the contact resistance. Zhou et al. [128] introduced an interfacial layer of MoO₃ to allow for highly competent charge separation and to suppress carrier reorganization. The PSCs exhibited a fairly high PCE of 14.05% with an FF of 81.5%. Zong et al. [129] introduced a simple synthetic and efficient MoO₂/N-doped carbon nanospheres complex inorganic HTL to establish a high capability and steady CsPbBr₃ PSCs. Xue et al. [130] used dopamine (DA) doping to improve the HTL work function and increase the perovskite film crystallinity. Ding et al. [131] modified a polyvinyl acetate with a carbonyl group at the boundary surface of CsPbBr₃/carbon to inactivate the perovskite surface defect states and intensify the energy level alignment between the CsPbBr₃ valence band and the carbon work function. Yang et al. [132] found that tris(N,N,N-tributyl-1-butanaminium)[[2,2′′6′ ,2′′-terpyridine] -4,4′,4 ′′—tricarboxylato(3−)-N1,N1′,N1′′]tris(thiocyanato-N)hydrogen ruthenate(4−) (N749) between the Cs-NiOx and CsPbIBr₂ can inhibit the phase separation and block moisture penetration. The inverted CsPbIBr₂ PSCs treated by N749 had amazing humidity stability. Zhu et al. [133] found that the diazonium atoms embracing the unpaired electrons in N,N’-Dicyclohexylcarbodiimide (DCC) have a strong passivation effect on the unpaired Pb²⁺ and Cs⁺ ion drawbacks, which greatly reduced the drawback state of CsPbBr₃ films and caused the non-radiation reorganization. Du et al. [134] drafted (R)-(-)-1-cyclohexylethylamine iodide (R-CEAI) to inactivate the deficiencies of perovskite, and grew a quasi-2D Ruddlesden–Popper perovskite on the 3D perovskite. The R-CEAI-served 2D/3D PSCs had a PCE of 22.52%. Xu et al. [135] constructed a PbS/CdS heterojunction in CsPbI_1.5Br_1.5 and the carbon electrode to perfect the PSCs stability of the device. Zou et al. [136] passivated the CsPbBr₃/carbon interface by using NiO nanocrystals. The obtained CsPbBr₃ films showed prominent physical and chemical properties.

Some groups even considered both the perovskite/ETL and perovskite/HTL interfaces. Liao et al. [137] added carbon quantum dots to the CsPbBr₃/TiO₂ interfaces and red phosphorus quantum dots to the CsPbBr₃/Carbon interfaces, which accelerated both electron and hole transfer into the interface layer. As a result, the Voc was increased by about 0.2 V. CsPbBr₃/CsSnBr₂I QDs bilayers [138], CsPbBr_3/CdZnSe@ZnSe QDs bilayers [139], and CsPbI₂Br/CsPbI₃ QDs bilayers [140] were also used to reduce the E_loss. Chen et al. [141] enhanced the morphology of CsPbIBr₂, PCE, and stability by introducing rubidium acetate (RbAc) to the ETL/perovskite/HTL interfaces. Shi et al. [142] synthesized two kinds of C₃N₄ materials (w-CN and y-CN) simultaneously and employed them in the two-sided boundary surface of the perovskite film. Table 3 summarizes the performances of PSCs based on interface engineering. The properties of the perovskite film were optimized, and the PCE was increased. Interface engineering can improve the transmission of charge between the interface of PSCs, reduce recombination loss, and improve the stability, which is an effective method to promote the photoelectric performance and long-term stability at the same time [143].

3. Results

Maximizing the PCE and improving the stability of all-inorganic CsPbX₃ perovskite solar cells is still a major challenge. We summarized some methods here. First, introducing additives such as X-site anions, B-site cations, HI, HPbI₃, precursor materials, and quantum dots could improve the crystallinity and morphology of the perovskite film. Choosing the appropriate radius for the addition was important, as was the molar ratio of the addition. Second, the proper solvent was helpful to enhance the properties of perovskite for excellent PSCs. To adapt to the future market demand, green solvents were popular. Third, interface modification could improve the film surface morphology and crystallinity. The charge transfer between layers was directly related to the PSCs’ performance. The heterojunction will be one of the future trends. PCE, long-term stability, and preparation cost are important evaluation indices of solar cells. There is no doubt that all-inorganic PSCs have infinite potential and broad application prospects. However, compared with organic–inorganic hybrid PSCs, the PCE of all-inorganic PSCs still has a certain gap. Some existing problems and research prospects of all-inorganic PSCs are summarized as follows: (1) the mechanism of all-inorganic PSCs have not been studied thoroughly until now. It was difficult to optimize the PSCs’ performance, ensure repeatability, and prepare them on a large scale. (2) There were inconsistencies in the evaluation of all-inorganic PSCs’ stability in reports. It may be necessary in the future to develop uniform evaluation criteria to better adapt to commercial applications. (3) The toxicity of lead was an unavoidable problem and may be studied in terms of lead leakage or replacement.

Author Contributions

Conceptualization, Y.C. and F.L.; validation, Y.C., F.L., M.Z. and Z.Y.; writing—original draft preparation, Y.C. and F.L.; writing—review and editing, Y.C.; visualization, Y.C.; supervision, Y.C.; project administration, Y.C.; funding acquisition, Y.C. All authors have read and agreed to the published version of the manuscript.

Institutional Review Board Statement

Not applicable.

Informed Consent Statement

Not applicable.

Data Availability Statement

No new data were created or analyzed in this study. Data sharing is available within the article.

Conflicts of Interest

The authors declare no conflict of interest.

Footnotes

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Figures and Tables

Figure 1. Four different structural phases of CsPbI3 and their phase transitions reprinted with permission from Ref. [39] 2018 American Chemical Society.

Figure 2. EAH-S method to grow CsPbI3 perovskite. (a) Schematic diagram of EAH-S method. AH: ammonium halide. (b) Photographs of the transitive films prepared from the precursor solutions with/without ammonium iodides and the corresponding films after soaking in EtOH. XRD patterns of the transitive films and the corresponding films after soaking in EtOH: (c) without ammonium iodides, (d) MAI, (f) BAI, and (g) DMAI. (e) PL position mapping of the transitive films after soaking in EtOH. PL intensity mapping of the transitive films and the corresponding films after soaking in EtOH: (h) MAI, (i) BAI, and (j) DMAI reprinted with permission from Ref. [112] 2022 Elsevier.

Figure 3. (a) Schematic of preparation process of CsPbI3 films with CsPbBr3 pieces. (b) Transmittance spectra of TiO2, TiO2/CsPbBr3 seeds, and TiO2/CsPbBr3 film. (c) Confocal PL intensity and (d) PL peak position maps of TiO2/CsPbBr3 pieces, respectively reprinted with permission from Ref. [126] 2023 Elsevier.

Table 1

Summary of various inorganic PSCs’ performance using additive engineering.

Additive		Device Configuration	Jsc(mA cm−2)	VOC (V)	FF	PCE (%)	Ref.
X site	Br−	FTO/TiO2/CsPbI2Br/CuBr2/Spiro-OMeTAD/MoO3/Ag	16.95	1.18	0.8	16.15%	[9]
	Br−	FTO/c-TiO2/m-TiO2/CsPbI2Br/Spiro-OMeTAD/Ag	11.89	1.11	0.75	9.84	[25]
	Br−	FTO/TiO2/CsPbI2.85Br0.15/PTAA/Au	19.75	1.135	0.766	17.17	[47]
	Br−	ITO/SnO2/LiF/CsPbI3-xBrx/Spiro-OMeTAD/Au	18.3	1.25	0.825	18.64	[48]
	Br−	ITO/SnO2/CsPbIxBr3-x/SIM/Spiro-OMeTAD/Au	18.01	1.27	0.79	18.06	[49]
	Cl−	FTO/TiO2/γ-CsPbI3:Cl0.03/PTAA/Ag	19.58	1.084	0.757	16.07	[51]
	SCN−	FTO/TiO2/CsPbI3/PTAA/Au	20.34	1.09	0.77	17.04	[52]
	SCN−	ITO/TiO2/CsPbBr3-1.5% NH4SCN/Spiro-OMeTAD/Au	7.76	1.375	0.793	8.47	[53]
B site	Sn2+	FTO/c-TiO2/CsPbI3/CuSCN/Au	10.05	0.85	0.59	5.12	[55]
	Ca2+	FTO/c-TiO2/m-TiO2/CsPbI3/P3HT/Au	17.9	0.94	0.8	13.5	[56]
	Sr2+	FTO/c-TiO2/m-TiO2/CsPb0.98Sr0.02I2Br/P3HT/Au	15.3	1.043	0.699	11.2	[57]
	Ba2+	ITO/SnO2/CsPbI3(α)/P3HT/Au	13.19	0.9	0.606	7.23	[59]
	Mn2+	FTO/TiO2/CsPbI3/PTAA/Au	19.53	1.1	0.77	16.52	[62]
	Cd2+	FTO/TiO2/CsPbIBr2-Cd2+/Carbon	11.53	1.324	0.696	10.63	[63]
	Bi3+	FTO/c-TiO2/CsPbI3(α)/CuI/Au	18.76	0.97	0.7259	13.21	[64]
	Sb3+	FTO/c-TiO2/CsPbI3/Spiro-OMeTAD/Au	13.15	1.04	0.67	9.4	[65]
	Yb3+	FTO/c-TiO2/CsPbI3(α)/Spiro-OMeTAD/Ag	18.4	1.13	0.6	12.4	[66]
	Eu3+	FTO/TiO2/CsPbI3(α)/Spiro-OMeTAD/Au	11.1	0.898	0.68	6.8	[67]
	In3+	FTO/c-TiO2/m-TiO2/CsPbI3/Carbon	15.68	1.2	0.64	12.04	[18]
	Er3+	ITO/NiO/CsI(PbBr2)0.97 (ErCl3)0.03/Nb2O5/Ag	12.36	1.34	0.705	11.61	[68]
	Gd3+	FTO/TiO2/CsPbI2Br0.96 (GdCl3)0.04/Spiro-OMeTAD/Au	16.09	1.222	0.825	16.24	[69]
HI		FTO/c-TiO2/CsPbI3 (γ)/P3HT/Au	16.53	1.04	0.657	11.3	[71]
HPbI3		FTO/c-TiO2/CsPbI3 (α)/Spiro-OMeTAD/Ag	14.53	1.15	0.71	11.86	[73]
HPbI3		FTO/c-TiO2/m-TiO2/CsPbI3(α)/Carbon	18.5	0.79	0.65	9.5	[74]
HPbI3		ITO/SnO2/CsPbI3/Spiro-OMeTAD/Au	16.59	1.07	0.7	12.4	[75]
HPbI3		FTO/TiO2/CsPbI3(γ)/PTAA/Au	18.95	1.059	0.751	15.07	[76]
HPbI3		FTO/c-TiO2/CsPbI3/Spiro-OMeTAD/Au	18.4	1.054	0.74	14.3	[77]
HPbI3		FTO/c-TiO2/CsPbI3(α)/Spi ro-OMeTAD/Ag	18.76	1.104	0.806	17.06	[23]
HPbI3		FTO/c-TiO2/CsPbI3(β)/Spiro-OMeTAD/Ag	20.23	1.11	0.82	18.4	[78]
H2PbI4		ITO/PTAA/CsPbI3/(C60/BCP)/Cu	17.10	1.12	0.7	13.4	[79]
DMAI		FTO/PEDOT:PSS/CsPbI3/(C60/BCP)/Ag	16.65	0.99	0.765	12.62	[80]
HI		FTO/c-TiO2/CsPbI3/PTAA/Au	21.15	1.062	0.77	17.3	[83]
DMAI		FTO/c-TiO2/m-TiO2/CsPbI3/Carbon	15.76	0.91	0.66	9.39	[84]
DMAI		FTO/c-TiO2/CsPbI3(β)/Spiro-OMeTAD/Ag	20.23	1.137	0.827	19.02	[29]
DMAI		FTO/c-TiO2/m-TiO2/CsPbI3(γ)/Spiro-OMeTAD/Ag	19.4	1.05	0.75	15.3	[85]
CsI		FTO/c-TiO2/m-TiO2/m-Al2O3/CsPbI3/Carbon	14.65	0.73	0.5	5.31	[86]
CsI		ITO/PTAA/CsPbI3(γ)/C60/BCP/Ag	17.8	0.96	0.73	12.5	[87]
CsI		ITO/SnO2/ZnO/CsPbI3/Spiro-OMeTAD/MoO3/Ag	18.84	1.09	0.8	16.39	[88]
CsBr		FTO/ZnO/CsPbI3-xBrx)/Carbon	19.1	0.96	0.68	12.39	[89]
HEMA		FTO/ZnO/CsPbI2Br/PM6/MoO3/Ag	15.81	1.23	0.83	16.13	[90]
MACl		FTO/c-TiO2/CsPbI3/spiro-OMeTAD/Au	20.59	1.198	0.825	20.37	[91]
CsPbBr3 QDs		ITO/SnO2/CsPbI3/CsPbBr3 QDs/spiro-OMeTAD/Au	18.02	1.09	0.821	16.17	[92]
ZnOX		ITO/SnO2/CsPb1−xSnxIBr2/Spiro-OMeTAD/Au	15.5	1.18	0.767	14.1	[93]
GuaSCN		FTO/c-TiO2/CsPbIBr2/Spiro-OMeTAD/Au	12.05	1.23	0.737	10.9	[94]

Table 2

Summary of various inorganic PSCs’ performance using solvent engineering.

Device Configuration	Jsc (mA cm−2)	VOC(V)	FF (%)	PCE(%)	Ref.
ITO/PEDOT:PSS/CsPbI2Br/PCBM/BCP/Al	10.9	1.06	-	6.8	[27]
FTO/NiOx/CsPbI2Br/ZnO@C60/Ag	15.2	1.14	0.77	13.3	[96]
ITO/c-TiO2/CsPbI2Br/Spiro-OMeTAD/Au	12.7	1.05	0.68	9.08	[97]
FTO/NiMgLiO/CsPbI2Br/PCBM/BCP/Ag	14.18	0.98	0.66	9.14	[98]
FTO/TiO2/CsPbI2Br/Spiro-OMeTAD/Au	15.33	1.2	0.79	14.78	[99]
FTO/TiO2/CsPbI3(α)/Spiro-MeOTAD/Ag	11.92	0.66	0.525	4.13	[100]
FTO/c-TiO2/CsPbBr3/Carbon	7.12	1.49	0.688	7.29	[101]
FTO/SnO2/CsPbIBr2/Carbon	10.15	1.19	0.563	6.79	[102]
FTO/c-TiO2/CsPbBr3/Carbon	7.48	1.51	0.845	9.55	[103]
FTO/c-TiO2/CsPbI2Br/Carbon	13.87	1.15	0.64	10.21	[104]
ITO/SnO2/CsPbI3/PEAI/Spiro-OMeTAD/MoO3/Ag	19.43	0.737	0.615	8.8	[105]
ITO/PEDOT:PSS/CsPbI3/PCBM/Al	18.66	1.05	0.733	14.4	[106]
ITO/SnO2/CsPbI3/Spiro-OMeTAD/Au	18.41	1.08	0.793	15.71	[24]
FTO/c-TiO2/CsPbBr3/carbon	6.46	1.34	0.68	5.86	[107]
ITO/SnO2/CsPbI2Br/PTAA/Au	14.6	1.162	0.791	14.31	[108]
FTO/Ni-TiO2/SnO2/CsPbBr3/CuPc/Carbon	8.24	1.31	0.814	8.79	[109]
FTO/NiOx/CsPbBr3/PC61BM/Ag	8.22	1.47	0.83	10.02	[110]
FTO/c-TiO2/CsPbIBr2/Spiro- OMeTAD/Ag	13.33	1.22	0.71	11.49	[111]
FTO/TiO2/CsPbI3/Carbon	18.7	1.075	0.764	15.35	[112]
FTO/TiO2/CsPbBr3/Carbon	8.51	1.31	-	8.25	[113]

Table 3

Summary of various inorganic PSCs’ performance using interface engineering.

Device Configuration	Jsc (mA cm−2)	VOC (V)	FF (%)	PCE (%)	Ref.
ITO/SnO2/ZnO/CsPbI2Br/Spiro-OMeTAD/MoO3/Ag	15	1.23	0.788	14.6	[116]
ITO/NiOx/CsPbI3/TiO2/ZnO/Ag	21.79	1.31	0.741	21.06	[117]
ITO/In2S3/CsPbIBr2/Sprio-OMeTAD/Au	7.76	1.09	0.66	5.59	[118]
FTO/SnO2/TiO2/CsBr/CsPbIBr2/Carbon	10.91	1.273	0.66	9.31	[119]
ITO/ZnO/MgxZn1-xO/CsPbI2Br/PM6/MoO3/Ag	15.8	1.31	0.78	16.04	[120]
ITO/TiO2 CL@NaPA/CsPbI2Br/P3HT/MoO2/Ag	15.18	1.1	0.68	11.35	[121]
ITO/SnO2/CsPbIBr2/carbon	8.5	1.23	0.67	7	[122]
FTO/ZnO/PC60BM/CH3NH3PbI3−xClx/spiro-OMeTAD/Ag	23.2	1.08	0.67	17	[123]
ITO/SnO2/PEIE/CsPbIBr2/Spiro-OMeTAD/MoO3/Ag	11	1.29	0.786	11.2	[124]
FTO/CsAc@TiO2 NRs/CsPbI2.25Br0.75/Carbon	16.29	1.145	0.741	13.81	[125]
FTO/TiO2/CsPbBr3 seeds//CsPbI3/Spiro-OMeTAD/Ag	20.53	1.14	0.7946	18.6	[126]
FTO/NiOx/CsPbIBr2/Au	10.44	0.62	0.52	3.4	[127]
ITO/SnO2/CsPbI2Br/Spiro-OMeTAD/MoO3/Ag	15.4	1.12	0.815	14.05	[128]
FTO/c-TiO2/m-TiO2/CsPbBr3/(MoO2/NC)/Carbon	7.2	1.532	0.852	9.4	[129]
ITO/DA-PEDOT:PSS/perovskite/PCBM/PN4N/Ag	22	1.08	0.775	18.5	[130]
FTO/c-TiO2/m-TiO2/CsPbBr3/PVAc/GO/Carbon	7.41	1.553	0.828	9.53	[131]
FTO/Cs-NiOx/N749/CsPbIBr2/PC61BM/BCP/Ag	11.49	1.19	0.69	9.49	[132]
FTO/c-TiO2/m-TiO2/CsPbBr3/DCC/Carbon	7.79	1.611	0.81	10.16	[133]
FTO/TiO2/perovskite/R-CEAI/Spiro-OMeTAD/Au	23.42	1.195	0.805	22.52	[134]
FTO/TiO2/CsPbI1.5Br1.5/PbS&R-CdS/Carbon	13.47	1.315	0.771	13.65	[135]
ITO/SnO2/CsPbBr3/NiO NCs/Carbon	7.57	1.57	0.774	9.19	[136]
FTO/c-TiO2/m-TiO2/CsPbBr3/RPQD/Carbon	7.33	1.47	0.76	8.2	[137]
FTO/c-TiO2/m-TiO2/CsPbBr3/CsSnIBr2-QDs/Carbon	8.7	1.39	0.755	9.13	[138]
FTO/c-TiO2/m-TiO2/CsPbBr3/QDs/Carbon	7.25	1.498	0.796	8.65	[139]
FTO/TiO2/CsPbI2Br/CsPbI3-QDs/PTAA/Au	15.25	1.204	0.787	14.45	[140]
ITO/SnO2/RbAc/CsPbIBr2/RbAc/Spiro-OMeTAD/Ag	12.03	1.36	0.725	12.11	[141]
FTO/TiO2/w-CN/CsPbIBr2/y-CN	11.19	1.36	0.664	10.1	[142]

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