
Cite this article as: | Xu Zhao, Shoudeng Zhong, Shuqi Wang, Shaozhen Li, and Sujuan Wu, Potassium thiocyanate additive for PEDOT:PSS layer to fabricate efficient tin-based perovskite solar cells, Int. J. Miner. Metall. Mater., 30(2023), No. 12, pp.2451-2458. https://dx.doi.org/10.1007/s12613-023-2738-y |
The power conversion efficiency (PCE) of tin-based perovskite solar cells (TPSCs) has exceeded 14% [1]. This could be attributed to the inverted device can help to reduce Sn2+ oxidation, promote charge transfer, and inhibit carrier recombination [2]. Among various hole transport materials used in inverted TPSCs, poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) has drawn much attention due to its low-temperature process and high transmittance [3]. Although the commercialized PEDOT:PSS has high mobility, the high acidity (pH ≈ 2) and hydrophilicity of PEDOT:PSS erodes adjacent indium tin oxide (ITO) and perovskite layer, which is detrimental to device stability [4]. Furthermore, there is high carrier recombination rate at the PEDOT:PSS/perovoskite interface, which will hinder hole transfer and cause open-circuit voltage (Voc) loss [5]. In addition, the PEDOT and the redundant PSS chain can couple with each other, resulting in the heterogeneity of PEDOT:PSS structure and increase insulation and reduce electrical conductivity [4,6]. Therefore, PEDOT:PSS hole transport layers (HTLs) need to be further optimized.
A number of HTLs are tried to improve the photoelectrical performance of inverted TPSCs. Inorganic copper thiocyanate (CuSCN) and NiOx are used to replace PEDOT:PSS as new HTLs due to their better energy level alignment with perovskite layer and superior hole mobility [7–10]. In addtion, the strategy of reducing the acidity and hydrophilicity of PEDOT:PSS is an effective method to improve the PCE and stability of perovskite solar cells (PSCs). It is reported that the PEDOT:PSS solution diluted by deionized water can not only reduce cost but also mitigate the acid corrosion of PEDOT:PSS [5,9–10]. Han et al. [11] have tried to adjust the PSS-rich surface and reduce energy level mismatch by introducing polyethylene glycol into PEDOT:PSS, resulting in the PCE of 5.12% and better device stability. Chen et al. [12] have found that the inserted tetrafluoro-tetracyanoquinodimethane layer between perovskite and PEDOT:PSS film can form a hydrophobic interface. It can reduce energy loss and passivates trap states, resulting in the PCE of 8.11% and excellent device stability. It is also found that the the inserted 2-chloroethylamine layer between PEDOT:PSS and pervoskite film can contribute to resist the Sn2+ oxidation and tune the crystallization process of perovskite film in tin-lead mixed PSCs [13]. It is reported that doping PEDOT:PSS with D-sorbitol can form a dense film to prevent water vapor erosion, inhibit iodide ion migration, and supress charge recombination, resulting in the improved PCE and stability [14]. Furthermore, the increase of electrical conductivity in HTLs is also one of the non-negligible ways to improve the PCE of PSCs. Zhu et al. [3,15] have reported that urea and hydroxyurea-doped PEDOT:PSS can neutralize the acidity of PEDOT:PSS, improve electrical conductivity, and inhibit charge recombination. It is also noted that the PSS could be replaced by highly dispersive sulfonated acetone-formaldehyde (SAF) to form PEDOT:SAF films with high conductivity, outstanding hydrophobicity and stability [4]. Gong et al. [16] found that highly conductive polyethylene oxide can significantly promote hole extraction and collection in lead-based PSCs (LPSCs) when it is introduced into PEDOT:PSS. The modification of PEDOT:PSS layer by alkali metal salts such as potassium chloride, sodium citrate, and sodium benzenesulfonate can optimize microstructure and suppress charge recombination, leading to enhancing PCE in LPSCs [5,17–18]. Wang et al. [19] has found that the inserted potassium thiocyanate (KSCN) interlayer between PEDOT:PSS and perovskite film can promote perovskite crystallization and charge transport in the FA0.75MA0.25SnBrI2-based TPSCs. The results suggest that modifying PEDOT:PSS film by a interlayer to fabricate a high-quality PEDOT:PSS HTLs is a good strategy. However, it is hardly favored to improve the photoelectrical characteristics of PEDOT:PSS HTLs by adding alkali metal salts to the diluted PEDOT:PSS solution in FASnI3-based TPSCs.
To reduce the acidity and hydrophilicity of PEDOT:PSS and improve the PCE and stability of TPSCs, the KSCN additive has been introduced into the diluted PEDOT:PSS solution by di-water with a volume ratio of 1:1. The device structure is ITO/PEDOT:PSS with or without KSCN/PEA0.1FA0.9SnI3 with 20mol% GASCN/PCBM/PEI/Ag. At an appropriate KSCN concentration, KSCN-PSCs exhibit a champion PCE of 8.39%, which is better than that of the reference device (6.70%). The characterization results show that the KSCN addition can enhance the electrical conductivity of HTLs fabricated by the diluted PEDOT:PSS solution, improve the microstructure of perovskite film, promote carrier transport, inhibit charge recombination, and reduce hysteresis effect in TPSCs. For a simple comparison, two kinds of films/TPSCs are studied: Reference-film/PSCs and KSCN-film/PSCs correspond to the PEDOT:PSS films or TPSCs based on PEDOT:PSS without KSCN and with KSCN additive at the optimal concentration, respectively. Moreover, two kinds of perovskite films are discussed: Reference/PVK-film and KSCN/PVK-film correspond to the perovskite films deposited on Reference- and KSCN-film, respectively.
The KSCN (99.99%) is obtained from Aladdin. KSCN solutions with the concentration of 3, 5, 10, 15, and 30 mg·mL–1 were dissolved into the mixed solution of PEDOT:PSS and deionized water (1:1, vol/vol), respectively to prepare the modified PEDOT:PSS solution, marked as KSCN-solution. It was spin-coated on the cleaned ITO and annealed at 140oC for 15 min in ambient air to prepare KSCN-film. After that, they were transferred to N2 glovebox, and the area is 0.09 cm2. The composition of perovksite film is PEA0.1FA0.9SnI3 with 20mol% GASCN (gallium thiocyanate). Ultraviolet photoelectron spectroscopy (UPS) of Reference- and KSCN-film were measured by an Axis Supra from KRATOS. Other materials, fabrication processes of Ag electrode, HTLs, perovskite, PCBM and PEI layer, and characterizations were the same as previous reported work [20]. All the materials were not be further purified.
Fig. 1 presents the relationship between current density (J) and voltage (V) and PCE at different KSCN concentrations. Error bars have been added in Fig. 1(b). Detailed photovoltaic (PV) parameters are listed in Table 1. When the KSCN concentration is lower than 5 mg·mL–1, all parameters increase with the increase of concentrations. Then, the PCE decreases as the KSCN concentration further increases, which can be attributed to the worse properties of PEDOT:PSS layer. Therefore, 5 mg·mL–1 KSCN is employed to fabricate KSCN-film/PSC and KSCN/PVK-film in the following work.
KSCN concentrations / (mg·mL–1) | Voc / V | Jsc / (mA·cm–2) | FF | PCE / % |
0 | 0.62 | 18.00 | 0.60 | 6.70 |
3 | 0.64 | 18.12 | 0.69 | 8.00 |
5 | 0.66 | 18.42 | 0.69 | 8.39 |
10 | 0.62 | 18.31 | 0.64 | 7.26 |
15 | 0.61 | 18.26 | 0.61 | 6.79 |
30 | 0.62 | 14.75 | 0.60 | 5.49 |
Notes: FF represents fill factor. |
The scanning electron microscopy (SEM) images of Reference- and KSCN-film are presented in Fig. 2(a)–(b). The similar images confirm that the KSCN addition can hardly influence the microstructure of PEDOT:PSS film. Fig. 2(c)–(f) shows the SEM imagesstructure and corresponding grain size distribution of Reference/PVK- and KSCN/PVK-film, respectively. As can be seen, the KSCN/PVK-film shows larger average grain size (244 nm) compared to that of the Reference/PVK-film (188 nm), which can benefit to promote carrier transport and collection in KSCN-PSCs [16–19], contributing to the enhanced PCE of KSCN-PSCs. Fig. 2(g)–(h) demonstrates the X-ray diffraction (XRD) patterns and the histograms of peak intensty and full-width-half-maximum (FWHM) of the (100) crystal plane in Reference/PVK- and KSCN/PVK-film, respectively. The diffraction peaks at 14.0° and 28.2° are assigned to (100) and (200) crystal planes, respectively [21]. Moreover, the intensity of (100) plane is stronger for KSCN/PVK-film than that of Reference/PVK-film, while the FWHM is adverse, and it decreases from 0.323° (Reference/PVK-film) to 0.301° (KSCN/PVK-film). The results confirm the improved microstructure in the KSCN/PVK-film [21–23].
The transmittance spectra of ITO, Reference-, and KSCN-film have been characterized. As presented in Fig. 3(a), the Reference- and KSCN-film are almost similar, indicating that the addition of KSCN has hardly influence on the transmittance of PEDOT:PSS layer. In addition, the excessive PSS in PEDOT:PSS can act as an insulating dispersant, resulting in poor electrical conductivity and the enhanced energy barrier for hole transport [24–25]. Thus, the electrical conductivity and corresponding devices of Reference- and KSCN-film have been characterized (Fig. 3(b)). Compared with Reference-film, the slope of KSCN-film is larger, which indicates that KSCN-film has better electrical conductivity. This can help to promote hole collection and transfer, leading to the improved PCE in KSCN-PSCs [26]. Fig. 3(c)–(d) demonstrates the absorption spectra and corresponding bandgaps of Reference/PVK- and KSCN/PVK-film, respectively. Apparently, the absorption spectra of Reference/PVK- and KSCN/PVK-film are similar. Meanwhile, the bandgaps of Reference/PVK- and KSCN/PVK-film are 1.396 and 1.395 eV, respectively, confirming that KSCN additive does not change the absorption and bandgap of perovskite layer.
To explore the influence of KSCN addition on J–V performance of TPSCs, Fig. 4(a) presents J–V curves of KSCN- and Reference-PSC with champion PCE. The KSCN-PSCs shows a PCE of 8.39%. The photovoltaic parameters are 0.66 V, 18.42 mA·cm–2, and 0.69, respectively, while they are 6.70%, 0.62 V, 18.00 mA·cm–2 and 0.60 in Reference-PSCs, respectively. The increased PCE in KSCN-PSCs mainly comes from the enhanced Voc and FF, which maybe come from the improved microstructure and promoted carrier transport [17–19,27]. Furthermore, the influence of KSCN addition on hysteresis effect has been studied. Fig. 4(b) demonstrates the J–V curves of KSCN- and Reference-PSCs characterized under two different scanning directions. Table 2 lists the detailed PV parameters. Hysteresis index (HI) will be gotten from the formula (1) [20]:
Devices | Scanning direction | Voc / V | Jsc / (mA·cm–2) | FF | PCE / % |
Reference-PSCs | Forward | 0.62 | 18.00 | 0.60 | 6.70 |
Reverse | 0.63 | 15.70 | 0.50 | 4.94 | |
KSCN-PSCs | Forward | 0.66 | 18.42 | 0.69 | 8.39 |
Reverse | 0.64 | 17.57 | 0.63 | 7.08 |
HI=|PCEreverse−PCEforward|PCEreverse | (1) |
where PCEreverse and PCEforward is the PCE at the corresponding scanning direction, respectively. It is noted that there is still an obvious hysteresis effect in KSCN-PSCs. The exact reasons and mechanisms about PV hysteresis is still a controversial issue. Ionic migration, charge recombination, and imbalance of electron and hole mobility are possibly the major reasons of PV hysteresis [28–31]. Compared with the HI value of Reference-PSCs (0.350), KSCN-PSCs exhibits a much smaller HI (0.187). Here it can be ascribed to more efficient carrier collection and less charge recombination in KSCN-PSCs [32]. To confirm the dependability of J–V result, the distributions of PCE, Voc, Jsc, and FF for KSCN- and Reference-PSCs from 25 devices each types of TPSCs have been provided. As presented in Fig. 4(c)–(f), the Reference- and KSCN-PSCs show excellent repeatability. Moreover, the KSCN-PSCs demonstrate obviously high average Voc and FF, resulting in higher average PCE. Thus, these results confirm that KSCN-PSCs demonstrate superior PCE and less hrysteresis effect.
To better understand the improved PV performance in KSCN-PSCs, J–V curves have been measured. As presented in Fig. 5(a), the leakage current density of KSCN-PSCs is lower than that of Reference-PSCs. This originates from the suppressed back charge density and carrier recombination in KSCN-PSCs, which is beneficial to boost FF and Voc [33–35], which could well agreement with the enhanced FF and Voc. To investigate carrier transport process, electrochemical impedance spectra (EIS) for KSCN- and Reference-PSCs have been characterized in dark at a bias vlotage of 0.30 V. The solid line corresponds to the results fitted by the equivalent circuit. Dots are the measured data. The equivalent circuit is composed of contact resistance and sheet resistance of substrate (Rs), carrier transfer resistance (Rtra), and constant-phase angle element (CPE) [36], respectively. The semicircular curves of Nyquist plots are positively correlated with charge transport of TPSCs [37]. As can be seen in Fig. 5(b), the Rtra are 435 and 346 Ω in Reference- and KSCN-PSCs, respectively, indicating that it is conducive to facilitate charge transport for KSCN-PSCs, leading to the improved J–V performance [38]. This is well accordance with the J–V results, confirming that the promoted carrier transfer and inhibited charge recombination contribute to the improved J–V performance in KSCN-PSCs.
In order to investigate the effect of KSCN additive on energy level of PEDOT:PSS layer, the ultraviolet photo-electron spectroscopy (UPS) are measured and energy level alignment of ITO, Reference-, and KSCN-film are provided, as shown in Fig. 6. The binding energy cut-off edge (Ecut-off) are 16.38 and 16.92 eV for Reference-film and KSCN-film, respectively (Fig. 6(a)). Based on the formula (Ef = hv – Ecut-off, hv = 21.22 eV), the calculated Fermi levels (Ef) are 4.84 eV for Reference-film and 4.30 eV for KSCN-film film [39]. As shown in Fig. 6(b), the energy level difference between the valence band maximum (Ev) and Ef is 0.38 and 0.81 eV for Reference- and KSCN-film, respectively. Thus, the Ev for Reference- and KSCN-film are 5.22 and 5.11 eV, respectively. The schematic diagram of energy level alignment for ITO, Reference-, and KSCN-film is presented in Fig. 6(c). It is noted that the KSCN additive makes the energy level alignment match well, which can contribute to increase the Voc of KSCN-PSCs [39]. These are consistent with the J–V results.
The stability is a significant factor for large-scale applications of TPSCs [26]. Fig. 7(a) demonstrates the stability of unencapsulated Reference- and KSCN-PSCs placed at about 25oC under N2 conditions for 528 h. Error bars have been added. During stored for 528 h, the PCE of KSCN-PSCs is still over than the Reference-PSCs. While the PCE of Reference-PSCs is lower than that of its originnal value after stored for 168 h. This results confirm that KSCN-PSCs demosntrate better stability, attributing to the inhibited oxygen penetration [14] and the slow passivation of trap states [27,35]. Fig. 7(b)–(c) presents the water contact angles of fresh Reference- and KSCN-film are 21.5° and 29.6°, respectivley. This suggests that the KSCN additive can improve the hydrophobicity of PEDOT:PSS film, which is beneficial to reduce the erosion of water vapor, resulting in the improved stability of KSNC-PSCs [4].
The KSCN-film was fabricated by adding KSCN into the PEDOT:PSS solution diluted by di-water with a volume ratio of 1:1. The further characterizations demonstrate that the KSCN additive have little effect on the microstructure, light absorption and transmittance, and band gap of PEDOT:PSS film, but could improve the electrical conductivity of HTLs, the average grain size and crystallinity of perovskite layer, and modulate the energy level alignment of HTLs. Thus, KSCN-PSCs show higher PCE and less hysteresis effect than those of Reference-PSCs. The improved photovoltaic performance in KSCN-PSCs can be attributed to the inhibited carrier recombination and promoted charge transfer. This work provides an available strategy to fabricate a high-quality PEDOT:PSS HTLs by a diluted PEDOT:PSS solution for efficient pure TPSCs.
This work was sponsored by Guangzhou Basic and Applied Basic Research Foundation (No. 303523).
All authors declare that they have no conflict of interest.
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1. | Aman Paswan, Rajan Mishra, Alok Kumar Patel. Performance Analysis of Mg Doped CuAlO2 HTL Based Organic Perovskite Solar Cell. 2024 IEEE Students Conference on Engineering and Systems (SCES), DOI:10.1109/SCES61914.2024.10652282 |
KSCN concentrations / (mg·mL–1) | Voc / V | Jsc / (mA·cm–2) | FF | PCE / % |
0 | 0.62 | 18.00 | 0.60 | 6.70 |
3 | 0.64 | 18.12 | 0.69 | 8.00 |
5 | 0.66 | 18.42 | 0.69 | 8.39 |
10 | 0.62 | 18.31 | 0.64 | 7.26 |
15 | 0.61 | 18.26 | 0.61 | 6.79 |
30 | 0.62 | 14.75 | 0.60 | 5.49 |
Notes: FF represents fill factor. |
Devices | Scanning direction | Voc / V | Jsc / (mA·cm–2) | FF | PCE / % |
Reference-PSCs | Forward | 0.62 | 18.00 | 0.60 | 6.70 |
Reverse | 0.63 | 15.70 | 0.50 | 4.94 | |
KSCN-PSCs | Forward | 0.66 | 18.42 | 0.69 | 8.39 |
Reverse | 0.64 | 17.57 | 0.63 | 7.08 |