Decylammonium sulfate post-treatment for efficient hole-conductor-free printable perovskite solar cells with reduced voltage loss

doi:10.21203/rs.3.rs-4112771/v1

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Decylammonium sulfate post-treatment for efficient hole-conductor-free printable perovskite solar cells with reduced voltage loss

https://doi.org/10.21203/rs.3.rs-4112771/v1

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published 09 Oct, 2024

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Hole-conductor-free printable mesoscopic perovskite solar cells (p-MPSCs) have attracted widespread attention for their low cost, up-scalability, and exceptional stability. However, the high defect density of perovskite and the absence of interfacial barrier layer between perovskite and carbon electrode cause profound open-circuit voltage (V_OC) loss, which results in uncompetitive power conversion efficiency (PCE). Herein, an anion-cation synergy of decylammonium sulfate (DA₂SO₄) is utilized for suppressing V_OC loss of p-MPSCs via a facile post-treatment method. DA⁺ cations transform the perovskite adjacent to carbon electrode into wide-bandgap 2D perovskite for blocking electrons, while the SO₄²⁻ anions interact with undercoordinated lead centers for reducing defect density. As a result, the modified device delivers an enhanced PCE from 17.78–19.59%, with an improved V_OC from 0.98 V to 1.06 V. Meanwhile, the modified device without any encapsulation exhibits excellent moisture stability with the PCE remained almost 99% of the initial value after 528 h aging in 75% RH air at room temperature.

Physical sciences/Chemistry/Photochemistry/Solar cells

Physical sciences/Chemistry/Energy

Anion-cation synergy

decylammonium

sulfate

2D perovskites

electron blocking

defect passivation

printable perovskite solar cells.

The power conversion efficiency (PCE) of perovskite solar cell (PSCs) has rised from 3.8–26.1% in the past dozen years, which has drawn tremendous attention in photovoltaic (PV) community.^{1 2} At present, adapting this PV technology from laboratory stage to industrialization becomes urgent.^{3 4 5} From this respect, hole-conductor-free printable mesoscopic perovskite solar cells (p-MPSCs) based on carbon electrodes have noteworthy advantages for its low cost, outstanding stability, and upscaling feasibility.^{6 7}

The p-MPSC contains a mesoporous scaffold composed of a mesoporous titanium dioxide (mp-TiO₂) layer, a mesoporous zirconium dioxide (mp-ZrO₂) layer and a porous carbon electrode layer, with the perovskite absorber infiltrating in it.⁸ Up to now, the highest reported PCE of p-MPSCs is lower than that of conventional PSCs.⁹ This is because of the severe open circuit voltage (V_OC) loss in p-MPSCs, which is related to the high defect density on the suface of perovskite and the absence of interfacial electron blocking layer (EBL) between perovskite and carbon electrode.^{10 11 12}

Accordingly, various strategies for passivating surface defects or constructing interfacial barrier layers have been investigated in p-MPSCs. Multiple passivators such as polyacrylonitrile (PAN), 1-(2-Chloroethyl) piperidine hydrochloride (ClEP), 2-(methylthio) ethylamine hydrochloride were utilized to reduce the perovksite surface defects in p-MPSCs.^{13 14 15} Other materials like NiO_x, CoO₄, VO_x have been used as the EBL.^{16 17 18} However, these techniques only provide limited improvement in PV performance. Therefore, more efforts have been made to develop the strategy of forming defect passivation and EBL simultaneously through simple process, which could deliver further breakthroughs in device performance.¹⁹ Considerable researches have demonstrated that in-situ formation of 2D/3D heterojunctions by incorporation large-sized organic ammonium cations such as long chain alkylammoniums, phenylalkylammoniums and their derivatives can effectively reduce the surface defects, and efficiently block the electron back transfer. ^{20 21 22 23} Besides, surface modification with these large organic ammoniums commonly improves the moisture resistance of the perovskite.²⁴ More robust inorganic surface modification can be obtained by introducing strong Lewis base anion like SO₄²⁻, PO₄³⁻, WO₄²⁻, which can bond with surface undercoordinated lead ions and thus passivate these defective sites.^{25 26} Therefore, appropriate pairing of large organic cations with strong Lewis base anion can synergically boost the device performance and stability.

In this work, we conducted post-treatment of p-MPSCs with the decylammonium sulfate (DA₂SO₄). The decylammonium (DA⁺) cations reacted with surface perovskite to form a wide bandgap 2D perovskite which acts as an EBL between perovskite and carbon electrode. Meanwhile, the SO₄²⁻ anion reduced the surface defects of perovskite by interacting with undercoordinated lead ions. Such a synergy of cation and anion effectively suppressed the V_OC loss in p-MPSCs. As a result, the modified device delivers a champion PCE of 19.59% and an increased V_OC from 0.98 V to 1.06 V. In addition, the DA₂SO₄ treated device also exhibited excellent moisture stability, which is attributed to the hydrophobicity of 2D perovskite and the low water permeability of PbSO₄.

For the fabrication of the p-MPSC, a triple-layer mesoporous scaffold (mp-TiO₂/mp-ZrO₂/carbon) was first deposited on an FTO glass substrate by screen printing, and then the perovskite absorber was filled in it by drop casting. For the DA₂SO₄ treatment, the fabricated p-MPSC was soaked in DA₂SO₄ solution and annealed for an optimized period of time. To detect the crystal structure information in the devices before and after DA₂SO₄ treatment, X-ray diffraction (XRD) was employed. As shown in Fig. 1a, the untreated and treated devices both exhibit typical characteristic peaks of 3D perovskite at 13.97°, 28.23°, and 31.64°, corresponding to (110), (220), (310) crystal planes. For the treated device, additional peaks at 4.43°, 8.95° can be indexed to (002), (004) crystal planes of the 2D perovskite of DA₂A_n − 1Pb_nI_3n+1 (n = 1; A = Cs, MA or FA).²⁷ Besides, the peaks at 6.06°, 9.13°, and 12.23° can be indexed to (040), (060), and (080) crystal planes of another type of 2D perovskite of DA₂A_n − 1Pb_nI_3n+1 (n = 2).²⁸ The XRD results confirm the formation of 2D perovskites in the device after DA₂SO₄ treatment. To investigate the possible interaction between SO₄²⁻ and Pb²⁺ in the perovskite film, Fourier transform infrared spectroscopy (FTIR) and X-ray photoelectron spectroscopy (XPS) were employed. For an ideally symmetric SO₄²⁻ tetrahedron, it would exhibit a broad infrared characteristic peak at about 1100 cm^− 1, which originates from the triply degenerate v₃ band. In some case, the v₁ band would be slightly activated and comes forth at about 975 cm^− 1.²⁹ From Fig. 1b, the peaks at 1159, 1113, and 1034 cm^− 1 originate from the split v₃ band, and the peak at 1000 cm^− 1 originates from the activated v₁ band. The triple-split of v₃ band and the elevation of peak position of v₁ band suggest the SO₄²⁻ tetrahedron has been distorted, indicating a strong electrostatic interaction between SO₄²⁻ and Pb²⁺.³⁰ Besides, the infrared characteristic peaks at 2800 ~ 3000 cm^− 1 correspond to the -CH₂- in the long alkyl chains of the 2D perovskite.²⁵ From XPS spectra (Supplementary Fig. 1), the binding energy of the Pb 4f_7/2 and Pb 4f_5/2 state of the perovskite film decreases from 138.71 eV and 143.61 eV to 137.95 eV and 142.8eV after DA₂SO₄ treatment, which further indicates the interaction between Pb²⁺ and SO₄²⁻.³¹ Fig. 1c shows the cross-sectional scanning electron microscopy (SEM) image of the fabricated p-MPSC, the mp-TiO₂ and mp-ZrO₂ layers are compactly filled with perovskite. Based on the above results, the DA₂SO₄ can transform the perovskite adjacent to carbon electrode into wide-bandgap 2D perovskite, while the SO₄²⁻ anions can bond with lead ions to form PbSO₄ at grain boundaries of perovskite (shown schematically in Fig. 1d).^{24 25}

We then evaluate the variation in water resistance of the perovskite after DA₂SO₄ treatment by soaking the untreated and treated devices directly in water. As shown in Figs. 2a-f, the active area of the treated device remains black even after water soaking for one hour, while the untreated counterpart completely turns yellow. Besides, the same water soaking test was conducted on MAPbI₃ crystal powders without and with DA₂SO₄ treatment, which exhibits a consistent enhancement of water resistance (Supplementary Fig. 2). This is possibly due to the formation of 2D perovskite with hydrophobic nature and the protection from PbSO₄ after DA₂SO₄ treatment.^{25 32}

The energy level alignment in the p-MPSC is determined by combining ultraviolet-visible spectroscopy (UV-vis) and the ultraviolet photoelectron spectroscopy (UPS).³³ From full UV-vis spectra and tauc plot (Fig. 3a and Supplementary Fig. 3), both untreated and DA₂SO₄ treated perovskite films exhibit a cut-off at 1.56 eV, corresponding to the bandgap energy (E_g) of 3D perovskite. The energy level of the valence band for untreated and treated perovskite films are determined from their UPS spectra to be 5.65 eV and 5.6 eV, respectively (Figs. 3b-c). From the high energy region of tauc plot (Supplementary Fig. 4), compared with the untreated film, the treated film occurs a sudden increase due to the absorbance of 2D perovskite, corresponding to an E_g from 2.12 to 2.33 eV.¹² Based on these data, the energy level alignment of 3D perovskite/2D perovskite/carbon is obtained and shown schematically in Fig. 3d. For the untreated device, the electrons would back transfer to carbon electrode and cause charge recombination, which results in severe V_OC loss.³⁴ For the DA₂SO₄ treated device, the wide-bandgap 2D perovskite generated an energy barrier (0.82 eV) between 3D perovskite and carbon electrode, which can efficiently block electrons and inhibit charge recombination.³⁵

The possible influence of DA₂SO₄ treatment on trap density was further investigated by conducting space charge limited current (SCLC) measurement. Electron and hole traps in perovskite demonstrate long-lived and short-lived dynamics for trapping of charge carriers, respectively.^{36 37 38 39} As a result, energy loss due to non-radiative recombination through hole traps normally is much more prominent than through electron traps. Therefore, we focus on detecting hole trap density based on a FTO/c-NiO_x/mp-ZrO₂/carbon structure for restoring the state of perovskite in p-MPSC.⁴⁰ From dark current density-voltage (J-V) curves (Supplementary Fig. 5), the trap filling limit voltage (V_TFL) of the perovskite decreases from 0.77 V to 0.64 V after DA₂SO₄ treatment. V_TFL correlates with trap density n_t through the following relationship:⁴¹

$${V}_{TFL}=\frac{{n}_{t}e{d}^{2}}{2\epsilon {\epsilon }_{0}}$$

in which e, d, ε, and ε₀ stands for the elementary charge, thickness of perovskite absorber, relative dielectric constant of perovskite absorber, and vacuum permittivity, respectively. Based on this equation, the hole trap density is found to decrease from 6.39 × 10¹⁴ cm^− 3 to 5.31× 10¹⁴ cm^− 3 by DA₂SO₄ treatment, which indicates defect passivation ability of DA₂SO₄.⁴² PL measurements were further performed with a mp-ZrO₂/glass structure to investigate the charge recombination process in perovskite. As shown in Fig. 4a, the intensity of the static PL emission increases significantly after DA₂SO₄ treatment. The time-resolved PL (TRPL) demonstrates the average carrier lifetime (τ_ave) of perovskite increases from 0.279 µs to 0.954 µs after DA₂SO₄ treatment (Fig. 4b and Supplementary Table 1). The increased PL emission intensity and the extended 𝜏_ave both indicate the suppression of non-radiative recombination in perovskite after DA₂SO₄ treatment, and further confirm its defect passivation capability.⁴³ The carrier dynamics in the p-MPSCs were also investigated by electrochemical impedance spectroscopy (EIS). The DA₂SO₄ treated device exhibits a smaller semicircle in the high frequency region and a larger semicircle in the low frequency region in the EIS spectrum compared with the untreated counterpart (Fig. 4c), which suggests an acceleration of charge transfer and a suppression of recombination by DA₂SO₄ treatment, respectively.⁴⁴ Meanwhile, after DA₂SO₄ treatment, the transient photo voltage (TPV) decay time of the device increases from 0.53 ms to 0.81 ms (Supplementary Fig. 6), and the ideal factor (n) of the device derived from light-dependent V_OC measurement decreases from 1.70 to 1.48 (Fig. 4d). These results sufficiently indicates that the trap-assisted Shockley-Read-Hall recombination is reduced by DA₂SO₄ treatment.^{45 46} Mott–Schottky measurement was also conducted to investigate the built-in potential (V_bi) of p-MPSCs. After DA₂SO₄ treatment, the V_bi of the device is elevated from 0.825 V to 0.915 V (Supplementary Fig. 7), which can be attributed to improved energy level alignment and reduced defects by DA₂SO₄ treatment.⁴⁷ The enhanced V_bi contributes to V_OC improvement by boosting carrier separation and extraction of charge.⁴⁸

To investigate the impact of DA₂SO₄ treatment on the photovoltaic performance of p-MPSCs, the DA₂SO₄ treating time was first optimized by comparing the variations of photovoltaic parameters (Supplementary Fig. 8 and Table 2). From the result, treating for 4 mins can realize the highest PCE, owing to the significant improvement of V_OC and the slight growths of J_SC and FF. When the treating time exceeds 15 mins, the PCE begins to decrease, because the prolonged treatment would transform the perovskites in mp-TiO₂ and mp-ZrO₂ into 2D perovskites, which could severely hamper the light absorption and charge extraction, resulting in severely reduced J_SC and FF.⁴⁹ Statistic diagrams of the photovoltaic parameters of 20 devices before and after DA₂SO₄ treatment for 4 mins are displayed (Fig. 5a, Supplementary Fig. 9 and Table 2). The DA₂SO₄ treatment significantly increases V_OC from (0.968 ± 0.022) V to (1.026 ± 0.021) V, and slightly increases J_SC and FF. As a result, the PCE is improved from (17.02 ± 0.53) % to (18.43 ± 0.63) %. The J-V curves of the champion treated device and its pristine state are shown in Fig. 5b. The pristine device displays a V_OC of 0.98 V, a J_SC of 23.51 mA·cm^− 2, a fill factor (FF) of 0.77, and a PCE of 17.78%. After DA₂SO₄ treatment, the device shows a significantly enhanced V_OC of 1.06 V, J_SC of 23.69 mA·cm^− 2 and FF of 0.78, leading to a champion PCE of 19.59%. Besides, the external quantum efficiency (EQE) was measured (Supplementary Fig. 10). The integrated J_SC of the champion and pristine devices are 22.89 and 22.67 mA·cm^− 2, consistent with the result in J-V test. From the maximum power point tracking (Fig. 5c), the stabilized PCE of the champion and pristine devices are 19.45% and 17.50%, matching the PCE obtained from J-V test. Finally, to evaluate the humid stability, an untreated and a treated device were stored in a humid aging chamber (75% RH, room temperature) without any encapsulation. As shown in Fig. 5d, after aging for 528 h, the PCE of the treated device remains 99% of the peak value, while the untreated device only remains 86% of the peak value. The result indicates that DA₂SO₄ treatment also improved the humid stability of p-MPSC.

In summary, we demonstrate the effective strategy to minimize V_OC loss for efficient p-MPSCs by post treating the device with DA₂SO₄. The salt modulator presents synergy effect, in which DA⁺ cations transformed 3D perovskites adjacent to carbon electrode into wide-bandgap 2D perovskites for blocking electrons, and SO₄²⁻ anions interacted with lead centers to reduce the surface defect density of perovskite. In this way, V_OC loss is effectively suppressed, while the V_OC is encouragingly improved from 0.98 V to 1.06 V, which brought a high PCE of 19.59%. Our study demonstrates the effectiveness of anion-cation synergy of regulating perovskite surface trap density and energy level on achieving highly efficient and stable p-MPSCs.

Materials

Formamidinium iodide (FAI, 99.5%, GreatCell), Lead (II) iodide (PbI₂, 99.99%, TCI), lead chloride (PbCl₂, 98%, Aladdin), N,N-dimethyl formamide (DMF, 99.8%, Acros), dimethyl sulfoxide (DMSO, 99.7%, Acros), titanium diisopropoxide bis(acetylacetonate) (75 wt% in isopropanol, Aladdin), TiO₂ paste (NR30, GreatCell), decylamine (DA, 98%, Sigama-Aldrich), sulfuric acid (H₂SO₄, 98%, Sinopharm). Cesium iodide (CsI), Methylamine iodine (MAI), methylamine hydrobromide (MABr) were purchased from Xi'an Polymer Light Technology Corp. ZrO₂ paste, carbon paste, and FTO glasses were supplied by Hubei WonderSolar Co., Ltd. Unless otherwise specified, all the materials were directly used without any purification.

Precursor preparation

The CsFAMA-based perovskite solution was prepared by dissolving 0.013 g CsI, 0.0045 g MABr, 0.0112 g PbCl₂, 0.0318 g MAI, 0.1376 g FAI, 0.461g PbI₂ in a mixed solvent (640 ul DMF with 160 ul DMSO) and stirring at 50°C for 1 h. The chemical formula can be described as Cs_0.05FA_0.8MA_0.15PbI_0.96Br_0.04 (with excess 5% MACl). Besides, the DA₂SO₄ solution was prepared by pipetting certain amount of DA and H₂SO₄ in a mixed solvent (chlorobenzene: isopropanol = 5:1) for 10 mM concentration.

Device Fabrication

First, the FTO glasses were etched with femtosecond laser for constructing circuit patterns. Next, the FTO glasses were ultrasonically cleaned with detergent, deionized water, and anhydrous ethanol, each solvent for 10 mins, respectively. Then, a compact TiO₂ layer was deposited onto the FTO glass by spraying pyrolysis with titanium isopropoxide bis(acetylacetonate) precursor (mass ration = 1:8) at 450 ℃. The triple-layer mesoporous scaffold was deposited onto the compact TiO₂ layer by screen-printing mp-TiO₂ paste, mp-ZrO₂ paste and carbon paste one by one, in which mp-TiO₂ layer was sintered at 500°C for 40 mins, mp-ZrO₂ and carbon layers were sintered together at 400°C for 40 mins. After cooling down, the perovskite precursor was drop onto the carbon for infiltrating the mesoporous scaffold, and then it was annealed at 56°C in a chamber for 18 h. All the processes were conducted in humid room temperature air (25 ℃, 70% RH).

Treatment process

The fabricated device was first immersed with DA₂SO₄ solution in a culture dish, and then heated at 50 ℃ for a certain period of time (1, 2, 4, 8, 15, 30 mins). After that, the device was taken out and washed by chlorobenzene to remove unreacted DA₂SO₄. Last, it was annealed at 70 ℃ for 20 mins. The process was conducted in humid room temperature air (25 ℃, 70% RH).

Characterization

A Nova NanoSEM 450 type field emission scanning electron microscope was employed to obtain SEM images. An X’pert PRO type X-ray diffractometer was employed to obtain XRD patterns, using Cu Kα radiation under the condition of 40 mA and 40 kV, with a scanning range from 4° to 40° and a scanning speed of 8°/min. A VERTEX70 type infrared Fourier transform microscope was employed to obtain FTIR spectra. An Axis-Ultra DLD-600 W type X-ray photoelectron spectrometer was employed to obtain XPS spectra. A SolidSpec-3700 Shimadzu UV–vis–NIR type spectrophotometer was employed to obtain UV-vis spectra. An ultraviolet photoelectron spectrometer based on a Kratos Axis Ultra DLD system using He I excitation source (hν = 21.22 eV) was employed to obtain UPS spectra. A LabRAM HR800 type Raman microscope with a 532 nm excitation laser was employed to obtain steady-state PL spectra. A HORIBA Scientific DeltaPro type fluorimeter was employed to obtain TRPL result. A Newport 91192 type solar simulator was employed to generate a simulated AM 1.5G illumination of 100 mW·cm^− 2, and with a Keithley 2400 type digital source/meter, the J–V curves can be obtained by reverse scanning from 1.1 to − 0.1 V with a scanning rate of -20 mV·s^− 1. The light intensity depended V_OC plot was obtained by conducting J-V tests under 1, 0.8, 0.5, 0.3, and 0.1 of the light intensity of the AM 1.5G illumination, achieved by the filters. The active area of the device was estimated to be 0.8 cm², and a mask with a 0.1 cm² circular aperture was employed for all the J-V tests. Besides, the dark J-V curves of SCLC were obtained by scanning from 0 to 2 V with a scanning rate of 10 mV·s^− 1. A 150 W Oriel xenon lamp fitted with a Cornerstone 74004 type monochromator was employed as a monochromatic source for obtaining external quantum efficiency. A ZAHNER Zennium type electrochemical workstation was employed to obtain EIS spectra, Mott-Schottky plot, and TPV plot. For the EIS, a frequency ranging from 1 MHz to 100 mHz was adopted, with a bias of -0.6 V under dark condition, and for the Mott-Schottky measurement, a voltage range from − 0.2 V to 1.2 V was adopted, with a frequency of 20 kHz and a step of 10 mV.

Sample preparation

For the XRD sample, the p-MPSC devices were first fabricated, and then the DA₂SO₄ treatment was conducted (or not) on them, as the methods mentioned above. Last, the carbon layer of the device was mechanically removed with adhesive tape for reducing the diffraction intensity of carbon. For the XPS, UPS, UV-vis, FTIR samples, the perovskite precursor solution was first prepared as the above description. And then, a consecutive two-step spin coating method was adopted for fabricating the perovskite film. Specifically, 30 ul perovskite solution was first pipetted onto an ultraviolet/ozone treated substrate (1.5 cm×1.5 cm), then spun at 1000 rpm for 10 s and 6000 rpm for 30 s with the accelerations of 200 and 2000 rpm, respectively. During the second step, 60 µL anti-solvent chlorobenzene was dropped onto the spinning film. Last, the film was annealed at 100°C for 20 mins. For the DA₂SO₄ treated perovskite film, DA₂SO₄ solution was first pipetted onto the fabricated perovskite film to react for 30 s, and then the two-step spinning process was repeated without using chlorobenzene. Last, the film was annealed at 70°C for 10 mins. The processes were conducted in a N₂ glovebox at room temperature. For the PL sample, mp-ZrO₂/Carbon mesoscopic scaffold was first deposited onto the glass, and then the perovskite was deposited in it, next the DA₂SO₄ treatment was conducted (or not) on that, as the methods mentioned above. Last, the carbon layer of the device was mechanically removed with adhesive tape and polished with sandpaper.

Conflict of Interest

The authors declare no conflict of interest.

Author contributions

Zexiong Qiu contributed the idea, experimental design, experimental process and manuscript writing; Jiale Liu provided guidance on experimental design and manuscript writing.

Acknowledgments

The authors acknowledge financial support from the National Natural Science Foundation of China (grant nos. 52172198, 51902117, and 91733301). The authors thank the Analytical and Testing Center of Huazhong University of Science and Technology (HUST) for performing various characterization and measurements.

Data Availability Statement

Research data are not shared.

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Decylammonium sulfate post-treatment for efficient hole-conductor-free printable perovskite solar cells with reduced voltage loss

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