Fabrication Of Perovskite Solar Cells Research Articles

Modulating secondary growth of perovskite grains through residual solvent evaporation

Over the past decade, perovskite solar cells (PSCs) have attracted enormous attention due to their high performance. One key to fabricating high-quality perovskite films lies in controlling the volatilization rate of residual solvents during the annealing process. This study systematically investigates how different protective substrates affect the volatilization rate of residual solvent in perovskite films. By adjusting the direction and rate of evaporation, the supersaturation time of the solution was precisely controlled, leading to effective recrystallization of the grains. Concurrently, the annealing time was optimized to enhance film quality further. This optimization aimed to increase crystallinity, reduce defects, and thereby minimize non-radiative recombination centers. Implementing these methodologies, particularly the use of filter paper as a protective substrate during a 2-minute annealing process, significantly improved the fill factor (FF) and open-circuit voltage (VOC) of the PSCs. This led to a remarkable 5.26% improvement in power conversion efficiency (PCE) compared to control devices. The strategies employed in this work demonstrate significant potential in improving PSC film quality. This approach not only advances our understanding of film formation dynamics but also provides a practical guideline for future PSC fabrication.

Stress-induced phase stability and optoelectronic property changes in cesium lead halide perovskites

Over the past decade, the certified power conversion efficiency of perovskite solar cells (PSCs) has increased to 26.1%. However, phase instability originating from lattice strains, has limited their commercialization. Strains will inevitably be generated during the PSC fabrication and service process due to the “soft lattice” nature of halide perovskites. In particular, flexible PSCs are subjected to not only mechanical tensile and compressive loads, but also suffer from thermal stresses. In this study, strain-induced changes in the phase stability and the corresponding optoelectronic properties of CsPbI3−xBrx (CsPbI3, CsPbBr3, and CsPbI2Br) systems under tensile and compressive stresses were investigated using first-principles calculations. The results showed that compressive stresses reduce the bandgap value and increase the light absorption coefficient; thus, the optoelectronic performance is improved, whereas the light absorption coefficient decreases regardless of how the bandgap changes under tensile stresses. Moreover, under the same stress, the tensile strain value was twice that of the compressive strain, and the critical value of the transition from the cubic to tetragonal phase was lower, indicating that phase stability was worse under tensile stresses. Therefore, during the fabrication of PSCs, the tensile stress state should be adjusted to the compressive stress state, which is favorable for enhancing PSCs photovoltaic performance and phase stability. The results not only provide direct evidence of tensile and compressive strains influencing the phase stability and optoelectronic property changes in halide perovskites, but also highlight lattice-strain tailoring for the composition design, process optimization, and interface engineering of efficient and stable PSCs.

Porous PbBr2 films modulation by indium tribromide additive for the fabrication of SnO2-based CsPbBr3 perovskite solar cells

The achievement of complete conversion of PbBr2 films presents a significant challenge in the development of CsPbBr3 films with consistent growth, comprehensive coverage, and controllable components. To address this challenge, introducing a porous structure in the planar PbBr2 film is advantageous for facilitating the immersion of CsBr precursor, thereby reducing impurity phase formation and mitigating strain caused by the film volume expansion. In order to accomplish this, indium tribromide (InBr3) was employed as an additive and the InBr3(DMF)3 adduct was utilized to expedite the release of organic molecules in PbBr2(DMF), resulting in the transformation of planar PbBr2 film into porous structures. The growth orientation of PbBr2 crystals was altered by this transformation, effectively suppressing the generation of metallic Pb impurities in the film. Additionally, it not only optimizes the morphology of CsPbBr3 film but also reduces impurity phase. As a result, the InBr3:CsPbBr3 perovskite solar cell achieved an efficiency of 7.28 %. The majority of In3+ ions were concentrated near the buried interface between SnO2 and InBr3:CsPbBr3, leading to significant improvements in both non-radiative recombination defect states within the perovskite film and electron injection and collection capabilities within the device.

Efficient and Stable CuSCN-based Perovskite Solar Cells Achieved by Interfacial Engineering with Amidinothiourea.

Cuprous thiocyanate (CuSCN) emerges as a prime candidate among inorganic hole-transport materials, particularly suitable for the fabrication of perovskite solar cells. Nonetheless, there is an Ohmic contact degradation between the perovskite and CuSCN layers. This is induced by polar solvents and undesired purities, which reduce device efficiency and operational stability. In this work, we introduce amidinothiourea (ASU) as an intermediate layer between perovskites and CuSCN to overcome the above obstacles. The characterization results confirm that ASU-modified perovskites have eliminated trap-induced defects by strong chemical bonding between -NH- and C═S from ASU and under-coordinated ions in perovskites. The interfacial engineering based on the ASU also reduces the potential barrier between the perovskite and CuSCN layers. The ASU-treated perovskite solar cells (PSC) with a gold electrode obtains an improved power conversion efficiency (PCE) from 16.36 to 18.03%. Furthermore, after being stored for 1800 h in ambient air (relative humidity (RH) = 45%), the related device without encapsulation maintains over 90% of its initial efficiency. The further combination of ASU and carbon-tape electrodes demonstrates its potential to fabricate low-cost but stable carbon-based PSCs. This work finds a universal approach for the fabrication of efficient and stable PSCs with different device structures.

Investigating the influence of natural dye extracts from Ocimum gratissimum, Solanum melongena, Piper guineese, and their blend in the fabrication of perovskite solar cells

Perovskite solar cells (PSCs) represent a promising alternative to conventional silicon solar cells but face challenges like instability stemming from structural defects, environmental toxicity due to the selection of precursors and additives, and concerns regarding long-term reliability. To address these issues, we investigated the viability of cost-effective and eco-friendly PSCs by strategically incorporating natural dyes derived from indigenous plants, including Ocimum gratisimum, Solanum melongena, and Piper guineese, into the MAPbI3 perovskite crystal, using a two-step sequential drop-casting technique. The resulting perovskite films underwent comprehensive analysis for their structural, morphological, optical and elemental composition using an X-ray diffractometer (XRD), scanning electron microscopy (SEM), UV–visible spectrophotometer (UV–Vis) and energy dispersive X-ray microscopy (EDX). Performance evaluation was conducted through J-V curve analysis using a solar simulator. The XRD analysis revealed polycrystalline films with enhanced diffraction intensities corresponding to a hexagonal structure, and the UV–Vis analysis demonstrated substantial improvements in light absorption with improved optical properties. SEM studies provided crucial correlations between morphology and performance, with each sample exhibiting unique attributes, and EDX analysis confirmed essential elements within the films. The current density-voltage analysis demonstrated a 1.83 % power conversion efficiency (PCE) for the natural dye-doped device under air, surpassing the pristine device. This study advances the understanding of the synergies between natural dyes and perovskite materials, emphasizing their potential to enhance PSC efficiency. The findings underscore the considerations for designing and optimizing PSCs, paving the way for further exploration of natural dye-based approaches in sustainable photovoltaic technologies.

Vacuum-Processed Propylene Urea Additive: A Novel Approach for Controlling the Growth of CH3NH3PbI3 Crystals in All Vacuum-Processed Perovskite Solar Cells.

In this study, we present a novel method for controlling the growth of perovskite crystals in the vacuum thermal evaporation process by utilizing a vacuum-processable additive, propylene urea (PU). By coevaporation of perovskite precursors with PU to form the perovskite layer, PU, acting as a Lewis base additive, retards the direct reaction between the perovskite precursors. This facilitates a larger domain size and reduced defect density. Following the removal of the residual additive, the perovskite layer, exhibiting improved crystallinity, demonstrates reduced charge recombination, as confirmed by a time-resolved microwave conductivity analysis. Consequently, there is a notable enhancement in open-circuit voltage and power conversion efficiency, increasing from 1.05 to 1.15 V and from 17.17 to 18.31%, respectively. The incorporation of a vacuum-processable and removable Lewis base additive into the fabrication of vacuum-processed perovskite solar cells offers new avenues for optimizing these devices.

Passivating Defects via Retarding the Reaction Rate of FAI and PbI2 Enables Stable Perovskite Solar Cells.

The two-step sequential deposition strategy has garnered widespread usage in the fabrication of high-performance perovskite solar cells based on FAPbI3. However, the rapid reaction between FAI and PbI2 during preparation often leads to incomplete reactions, reducing the device efficiency and stability. Herein, we introduced a multifunctional additive, 2-thiophenyl trifluoroacetone (TTA), into the FAI precursor. The incorporation of TTA has proven to be highly effective in slowing the reaction rate between FAI and PbI2, resulting in increased perovskite formation and improved efficiency and stability of the devices. TTA's CF3 groups interact with FAI via hydrogen bonding, effectively suppressing FA+ defects. The S and C═O groups share lone pair electrons with uncoordinated Pb2+, leading to a reduction in perovskite film defects and suppressing nonradiative recombination. Additionally, the CF3 groups impart hydrophobicity, protecting the perovskite film from moisture-induced erosion. As a result, the TTA-modified perovskite film achieves a Champion efficiency of 23.42% compared to the control's 21.52, with 20.58% efficiency for a 25 cm2 solar module. Remarkably, the unencapsulated Champion device retains 86% of its initial PCE after 1080 h under dark conditions (60 ± 5 °C, 35 ± 5% RH), indicating enhanced long-term stability. These findings offer a promising and cost-effective tactic for high-quality perovskite film fabrication.

Broadband enhancement of SiO2@TiO2 light-trapping nanostructure for improving the efficiency of perovskite solar cells

High-efficiency perovskite solar cells (PSCs) are one of the promising candidates to solve the energy crisis worldwide. Optical loss is one of the factors limiting the efficiency of PSCs and antireflection layers provide a dependable method for improving the efficiency of PSCs. Here, a design and optimization of PSCs with a SiO2@TiO2 nanoparticles (NPs) antireflection layer is systematically studied by COMSOL Multiphysics. The effect of different shell-thickness ratios (STRs) on the average light absorption and short-circuit current density of PSCs is simulated and compared with that of planar PSCs. The results show that the average light absorption of PSCs with SiO2@TiO2 NPs of 0.08 STR is 83.21%, which is 5.17% higher than that of PSCs with SiO2 NPs and 10.11% higher than that of planar PSCs. Our results provide theoretical guidance for using SiO2@TiO2 NPs as antireflection layers in the fabrication of PSCs.

Anti-Solvent-Free Fabrication of Stable FA0.9Cs0.1PbI3 Perovskite Solar Cells with Efficiency Exceeding 24.0% through a Naphthalene-Based Passivator.

The anti-solvent-free fabrication of high-efficiency perovskite solar cells (PSCs) holds immense significance for the transition from laboratory-scale to large-scale commercial applications. However, the device performance is severely hindered by the increased occurrence of surface defects resulting from the lack of control over nucleation and crystallization of perovskite using anti-solvent methods. In this study, 2-(naphthalen-2-yl)ethylamine hydriodide (NEAI) is employed as the surface passivator for perovskite films without using any anti-solvent. Naphthalene demonstrates strong π-π conjugation, which aids in the efficient extraction of charge carriers. Additionally, the naphthalene-ring moieties form a tight attachment to the perovskite surface. After NEAI treatment, FA and I vacancies are selectively occupied by NEA+ and I- in NEAI respectively, thus effectively passivating the surface defects and isolating the surface from moisture. Ultimately, the optimized NEAI-treated device achieves a promising power conversion efficiency (PCE) of 24.19% (with a certified efficiency of 23.94%), featuring a high fill factor of 83.53%. It stands out as one of the reported high PCEs achieved for PSCs using the spin-coating technique without the need for any anti-solvent so far. Furthermore, the NEAI-treated device can maintain ≈87% of its initial PCE after 2000h in ambient air with a relative humidity of 30%±5%.

Record-Efficiency Printable Hole-Conductor-Free Mesoscopic Perovskite Solar Cells Enabled by the Multifunctional Schiff Base Derivative.

Tailoring multifunctional additives for performing interfacial modifications, improving crystallization, and passivating defects is instrumental for the fabrication of efficient and stable perovskite solar cells (PSCs). Here, a Schiff base derivative, (chloromethylene) dimethyliminium chloride (CDCl), is introduced as an additive to modify the interface between the mesoporous TiO2 electron transport layer and the MAPbI3 light absorber during the annealing process. CDCl chemically links to TiO2 and MAPbI3 through coordination and hydrogen bonding, respectively, and results in the construction of fast electron extraction channels. CDCl also optimizes the energy-level alignment of the TiO2/MAPbI3 heterojunction and improves the pore-filling and crystallization of MAPbI3 in the mesoscopic scaffold, which inhibits nonradiative recombination and eliminates open-circuit voltage losses. As a result, an impressive power conversion efficiency of 19.74%, which is the best one ever reported, is obtained for printable carbon-based hole-conductor-free PSCs based on MAPbI3.

Unraveling the Influence of Solvent on Side Reactions between Formamidinium Lead Triiodide and Methylammonium Cations.

Formamidinium lead triiodide (FAPbI3) perovskite thin films are commonly deposited through a solution process, often incorporating a specific amount of methylammonium halide to stabilize the α-phase or enhance their crystallinity. The precursor solution for such coatings significantly influences the fabrication of perovskite solar cells (PSCs), involving time-dependent aging and byproduct formation. The chemical principle underlying this behavior is believed to be related to the deprotonation of methylamine cations (MA+) and subsequent chemical reactions with FA+ to generate N-methylformamidinium. Nevertheless, the role of the solvent in the side reactions between these organic cations remains unclear. This work systematically investigates the reaction reactivity in three protic solvents and three aprotic solvents. We uncover the hidden role of dimethylamine from the hydrolysis products of N,N-dimethylformamide, promoting the reaction between FA+ and MA+. Additionally, we elucidate the impact of environmental factors, such as water and oxygen, in stabilizing precursor solutions. This work establishes a basic concept and scientific direction for rationalizing high-efficiency, reproducible, and long-term-stable PSCs.

Fluorination of Star‐Shaped Cyclopenta[2,1‐b;3,4‐b′]dithiophene Derivatives and Its Application as Hole‐Transporting Materials in Scalable Perovskite Solar Cell Fabrication by Bar Coating

Fluorination of Star‐Shaped Cyclopenta[2,1‐b;3,4‐b′]dithiophene Derivatives and Its Application as Hole‐Transporting Materials in Scalable Perovskite Solar Cell Fabrication by Bar Coating

Enhancing performance of two‐step fabricated perovskite solar cells with sulfonium triflate‐based additive

AbstractWe incorporated triphenylsulfonium triflate (TPST), a sulfonium‐based additive consisting of polar triflate and bulky hydrophobic phenyl rings, to the PbI2 precursor solution for preparation of less‐defect perovskite film via two‐step fabrication. TPST induced localized alterations in the array of the PbI2 structure due to its large size, thereby forming a more discontinuous and coarser surface with a greater number of pinholes and subsequently facilitating more efficient organic–inorganic reactions. As a result, we achieved the production of thick perovskite films with enlarged granules and decreased PbI2 residuals in the two‐step fabrication process. Furthermore, TPST facilitated the passivation of bulk film defects by increasing the binding energy with the defects. Consequently, the ITO/SnO2 np‐based device and the FTO/CBD SnO2‐based device obtained the best PCEs of 23.88% and 24.30%, respectively. Furthermore, the moisture stability of the perovskite was improved by the hydrophobic character of the TPST additive.image

Fabricating Planar Perovskite Solar Cells through a Greener Approach.

High-quality perovskite thin films are typically produced via solvent engineering, which results in efficient perovskite solar cells (PSCs). Nevertheless, the use of hazardous solvents like precursor solvents (N-Methyl-2-pyrrolidone (NMP), dimethyl sulfoxide (DMSO), dimethylformamide (DMF), gamma-butyrolactone (GBL)) and antisolvents (chlorobenzene (CB), dibutyl ether (DEE), diethyl ether (Et2O), etc.) is crucial to the preparation of perovskite solutions and the control of perovskite thin film crystallization. The consumption of hazardous solvents poses an imminent threat to both the health of manufacturers and the environment. Consequently, before PSCs are commercialized, the current concerns about the toxicity of solvents must be addressed. In this study, we fabricated highly efficient planar PSCs using a novel, environmentally friendly method. Initially, we employed a greener solvent engineering approach that substituted the hazardous precursor solvents with an environmentally friendly solvent called triethyl phosphate (TEP). In the following stage, we fabricated perovskite thin films without the use of an antisolvent by employing a two-step procedure. Of all the greener techniques used to fabricate PSCs, the FTO/SnO2/MAFAPbI3/spiro-OMeTAD planar device configuration yielded the highest PCE of 20.98%. Therefore, this work addresses the toxicity of the solvents used in the perovskite film fabrication procedure and provides a promising universal method for producing PSCs with high efficiency. The aforementioned environmentally friendly approach might allow for PSC fabrication on an industrial scale in the future under sustainable conditions.

Slot‐Die Deposition of CuSCN Using Asymmetric Alkyl Sulfides as Cosolvent for Low‐Cost and Fully Scalable Perovskite Solar Cell Fabrication

The development of industrially relevant deposition processes for efficient, stable, and inexpensive charge extracting layers is crucial for the commercialization of perovskite solar cells (PSCs). This work demonstrates, for the first time, the deposition of copper thiocyanate (CuSCN) as a low‐cost and reliable hole‐transport layer using slot‐die coating. Methyl ethyl sulfide is thereby used as an asymmetric cosolvent to significantly increase the solubility of CuSCN in the utilized slot‐die ink compared to traditional pure diethyl sulfide‐based solutions. Optimized CuSCN inks allow for the deposition of CuSCN layers on 5 × 10 cm2 substrates with a wide range of thicknesses. Multidimensional imaging photoluminescence techniques are used to investigate the uniformity of the CuSCN thin films deposition as well as the influence of the solvent on charge losses. Finally, the CuSCN slot‐die deposition is integrated into a fully upscalable PSC fabrication process showing 19.1% power conversion efficiency for small laboratory cells and 14.7% for 9 cm2 minimodules. Furthermore, semitransparent minimodules retain 80% of their initial efficiency after 500 h of constant illumination.

MXene‐Based Energy Devices: From Progressive to Prospective

AbstractEvery once in a while, a revolutionary technological development arises, which leads to a significant change in the way to approach research and push development efforts. The appetite for new technology compels society to look for game‐changing materials, that can transform the industry and make advances. Sustainable energy production is paramount to addressing the climate crisis, and energy generation and storage play an important role in the development of self‐powered microelectronic devices. The 2D materials, MXenes have emerged as promising candidates for energy and other applications owing to their inherent electrical merits, high specific surface area, and tunable properties. Particularly, in the context of additive and interfacial materials for perovskite solar cell fabrication and utilization as additives in secondary batteries, this review delves into the application of MXenes in such devices. The protocols of MXenes and their nanostructures tailoring toward such applications and, the underlying mechanism is uncovered. Further, the existing challenges and direction for future in MXene‐based energy harvesters are discussed.

A Hole-Selective Self-Assembled Monolayer for Both Efficient Perovskite and Organic Solar Cells.

Self-assembled monolayers (SAMs) emerging as promising hole-selective layers (HSLs) are advantageous for facile processability, low cost, and minimal material consumption in the fabrication of both perovskite solar cells (PSCs) and organic solar cells (OSCs). However, owing to the different nature between perovskites and organic semiconductors, few SAMs were reported to effectively accommodate both PSCs and OSCs at the same time. In this regard, a universally applicable SAM that can accommodate both perovskites and organic semiconductors could be desirable for simplifying cell manufacturing, especially from an industrial perspective. In this work, we designed a SAM, TDPA-Cl by introducing chlorinated phenothiazine as the headgroup and linking with anchor phosphonic acid through a butyl chain. The resulting dense SAM was carefully characterized in terms of molecular bonding, surface morphology, and packing density, and its functions in OSCs and PSCs were discussed from the aspects of interactions with the absorber layer, energy level alignment, and charge-selective dipoles. The PM6:Y6-based OSCs with TDPA-Cl SAM as the HSL showed a superior performance to those with PEDOT:PSS. Furthermore, the universality was proved with an efficiency of 17.4% in the D18:Y6 system. In PSCs, the TDPA-Cl-based devices delivered a better performance of 22.4% than the PTAA-based devices (20.8%) with improved processability and reproducibility. This work represents a SAM with reasonably good compromise between the differing requirements of OSCs and PSCs.

Theoretical investigation of triphenylamine/anthradithiophene based systems as potential organic hole transport materials for perovskite solar cells

Hole transport materials (HTMs) are important constituents in perovskite solar cell fabrication. In this work structure property relationship of five different HTMs based on triphenylamine/anthradithiophene systems are investigated using DFT method. The orientation of the attachment of the thiophene rings on the anthracene core of anthradithiophene system has significant effect on the electronic and optical properties of the HTMs. The results are compared with the well-known HTMs. The predicted hole mobility of the molecules are found to be similar order of magnitude as that of spiro-OMeTAD. Thus, these HTMs can be potential replacements for spiro-OMeTAD in perovskite solar cell applications.

Fluorination of Star‐Shaped Cyclopenta[2,1‐b;3,4‐b′]dithiophene Derivatives and Its Application as Hole‐Transporting Materials in Scalable Perovskite Solar Cell Fabrication by Bar Coating

In this study, three novel star‐shaped small molecules HYC‐oF, HYC‐mF, and HYC‐H are designed and synthesized and are applied in perovskite solar cells (PSCs) as efficient hole‐transporting materials (HTMs). Compared with non‐fluorinated HYC‐H, F‐substituted analogs HYC‐oF and HYC‐mF exhibited enhanced hole mobility, suitable energy level alignment, improved interfacial contact and hole extraction/transport capability, better passivation effect, as well as increased hydrophobicity. PSC fabrication by spin‐coating this series of HYC‐oF, HYC‐mF, and HYC‐H molecules on a bar‐coated perovskite layer yielded PCEs values of 19.64%, 18.38%, and 16.98%, respectively. In order to realize a fully scalable PSC preparation process, sequential coating of HYC‐oF layer on perovskite layer all by thermal‐assisted bar‐coating (TABC) method was carried out on 10 × 10 cm2 area. The TABC‐based HYC‐oF layer had a compact and uniform morphology with full surface coverage on the TABC‐based perovskite film. Under optimized condition, the PSCs fabricated from such film exhibited a PCE of 18.49% as compared with a lower power conversion efficiency (PCE) of 17.51% from the reference cell using TABC‐based spiro‐OMeTAD. This work demonstrates the potential of fluorinated star‐shaped cyclopenta[2,1‐b;3,4‐b′]dithiophene (CPDT)‐based molecule as HTM for achieving efficient PSC in both small and large scale.

Green Solvent Strategies toward Sustainable Perovskite Solar Cell Fabrication

The shift towards ecofriendly solvents in perovskite solar cell (PSC) production represents a significant leap towards sustainable renewable energy generation, effectively addressing concerns related to the harmful nature of conventional solvents employed in PSC manufacturing. This review assesses the toxicity of traditional solvents utilized in the PSC fabrication process as well as recent studies and challenges related to substituting toxic solvents with less harmful or green alternatives. Although considerable efforts have been made to adopt greener solvents, this review underscores the variations in evaluations based on specific criteria, highlighting the need for thorough consideration to ensure the viability and sustainability of each solvent replacement. This study offers a comprehensive exploration of the transition to greener solvents in PSC fabrication and elucidates the associated challenges and opportunities in this pivotal shift towards a more environmentally sustainable approach to renewable energy production.