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Deep insights into interface engineering by buffer layer for efficient perovskite solar cells: a first-principles study; é?????é??é??????¤aé?3è????μ?±???-?????2?±????é?￠?·￥?¨?????·±??￥???è§￡: ????????§????????????;
摘要： Recent years have seen swift increase in the power conversion efficiency of perovskite solar cells (PSCs). Interface engineering is a promising route for further improving the performance of PSCs. Here we perform first-principles calculations to explore the effect of four candidate buffer materials (MACl, MAI, PbCl2 and PbI2) on the electronic structures of the interface between MAPbI3 absorber and TiO2. We find that MAX (X = Cl, I) as buffer layers will introduce a high electron barrier and enhance the electron-hole recombination. Additionally, MAX does not passivate the surface states well. The conduction band minimum of PbI2 is much lower than that of MAPbI3 absorber, which significantly limits the band bending of the absorber and open-circuit voltage of solar cells. On the other side, suitable bandedge energy level positions, small lattice mismatch with TiO2 surfaces, and excellent surface passivation make PbCl2 a promising buffer material for absorber/electron-transport-layer interface engineering in PSCs. Our results in this work thus provide deep understanding on the effects of interface engineering with a buffer layer, which shall be useful for improving the performance of PSCs and related optoelectronics.
关键词： perovskite solar cells,band alignment,interfacial defect passivation,buffer layer,interface engineering
更新于2025-09-23 15:21:01
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<i>In situ</i> study of the film formation mechanism of organica??inorganic hybrid perovskite solar cells: controlling the solvate phase using an additive system
摘要： As a coating method compatible with printing, one-step spin-coating is widely used for fabricating perovskite thin films. Controlling the crystal growth rate of two precursors is essential to obtain a homogeneous film morphology. However, the film formation mechanism and role of solvate systems during spin-coating have not yet been clearly revealed. In this work, we implemented the in situ grazing incidence wide-angle X-ray scattering of CH3NH3PbI3 perovskite material based on various additive systems to adjust the unbalanced crystal growth rate of CH3NH3I and PbI2. As we expected, the behavior of the solvate phase was strikingly mediated by various additives, and one of the additives greatly slowed the PbI2 solvate phase, thus overcoming the imbalance in the crystal growth rate. Consequently, the well-controlled perovskite films have both good film morphology and high photovoltaic performance with excellent reproducibility.
关键词： in situ study,solvate phase,perovskite solar cells,film formation mechanism,additive system
更新于2025-09-23 15:21:01
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Green Solution Bathing Process for Efficient Large-area Planar Perovskite Solar Cells
摘要： Perovskite solar cells (PSCs) towards practical application relies on high efficiency, long lifetime, low toxicity and device upscaling. To realize large-area PSCs, a green solution bathing strategy is delivered to prepare high-performance PSCs. By utilizing 2-pentanol as a green solvent and formamidinium chloride (FACl) as a solute in the green solution bathing, perovskite films with enlarged grain sizes, improved crystallinity and alleviated defect state density were obtained, resulting in the enhancement in the power conversion efficiency of PSCs. Coupled with 2-pentanol and FACl, a champion efficiency of 21.03% for small cells (0.103 cm2) and over 18% for large size (1.00 cm2) were obtained based on the GSB process, which can outperform its counterpart made from commonly-used anti-solvent dropping method. In addition, a large perovskite film (5 cm × 5 cm) with obvious mirror effect was successfully prepared. Our innovative approach paves the way to promote device upscaling of PSCs via environment-friendly technique.
关键词： 2-pentanol,green solvent,large-area,solution bathing,perovskite solar cells,FACl
更新于2025-09-23 15:21:01
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Designing Large Area Single Crystal Perovskite Solar Cells
摘要： Organic-inorganic halide single-crystal perovskite solar cells (PSCs) are promising for higher efficiency and better stability, while their development lags far behind polycrystalline counterpart. In particular, low efficiency (<5%) of large-area devices makes it challenging to be an alternative perovskite photovoltaic technology. In this perspective, we highlight the optimization of crystal growth and reduction of crystal thickness are keys to improve performance of the large-area single-crystal PSCs. After analyzing the characteristics of perovskite crystal growth methods and efficiency evolution of single-crystal PSCs, we conclude the low efficiency of large-area devices is due to conflict between low crystal quality and large crystal thickness. Then, we propose methods to grow high-quality perovskite single crystals and possible strategy to reduce the crystal thickness. Finally, investigation of key factors and exploration of large-area application are suggested to be conducted in parallel for future development of single-crystal PSCs.
关键词： large area,perovskite solar cells,single crystal,thickness reduction,crystal growth
更新于2025-09-23 15:21:01
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Using soft polymer template engineering of mesoporous TiO <sub/>2</sub> scaffolds to increase perovskite grain size and solar cell efficiency
摘要： The mesoporous (meso)-TiO2 layer is a key component of high efficiency perovskite solar cells (PSCs). Herein, pore size controllable meso-TiO2 layers are prepared using spin coating of commercial TiO2 nanoparticle (NP) paste with added soft polymer templates (SPT) followed by removal of the SPT at 500 °C. The SPTs consist of swollen crosslinked polymer colloids (microgels, MGs) or a commercial linear polymer (denoted as LIN). The MGs and LIN were comprised of the same polymer, which was poly(N-isopropylacrylamide) (PNIPAm). Large (L-MG) and small (S-MG) MG SPTs were employed to study the effect of template size. The SPT approach enabled pore size engineering in one deposition step. The SPT/TiO2 nanoparticle films had pore sizes > 100 nm; whereas, the average pore size was 37 nm for the control meso-TiO2 scaffold. The largest pore sizes were obtained using L-MG. SPT engineering increased the perovskite grain size in the same order as the SPT sizes: LIN < S-MG < L-MG and these grain sizes were larger than obtained using the control. The power conversion efficiencies (PCEs) of the SPT/TiO2-devices were ~ 20% higher than that for the control meso-TiO2 device and the PCE of the champion S-MG device was 18.8%. The PCE improvement is due to the increased grain size and more effective light harvesting of the SPT devices. The increased grain size was also responsible for the improved stability of the SPT/TiO2 devices. The SPT method used here is simple, scalable and versatile and should also apply to other PSCs.
关键词： Perovskite solar cells,template engineering,mesoporous TiO2,porosity,microgel,grain size.
更新于2025-09-23 15:21:01
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Highly Efficient and Stable Pure 2D Perovskite Based Solar Cells with 3-Aminopropionitrile Organic Cation
摘要： Pure two-dimensional (2D) perovskite (n = 1) based perovskite solar cells (PSCs) have been proven to have excellent stability against humidity, but the photovoltaic performance is very poor due to the parallel orientation to the substrate and mismatched energy alignment in the PSC device. We report herein a novel bulky organic cation of 3-aminopropionitrile (3-APN) for constructing a pure 2D hybrid lead-iodide perovskite. The crystal structure of (3-APN)2PbI4 features a stable layered and undistorted PbI6 octahedral geometry ( ∠ Pb–I–Pb = 180o) with a small I···I distance (4.66 ?), and the crystals grow in a dominant out-of-plane direction to the substrate. In addition, the existence of intramolecular H-bond between cyano groups and ammonium heads result in an appropriate valence band level of (3-APN)2PbI4 for well-matched energy level alignment in the device, benefitting the interfacial charge transfer and hence better photovoltaic performance. As a result, the PSC with the pure 2D (3-APN)2PbI4 perovskite based PSC achieves power conversion efficiency of 3.39%, which is the highest value thus far for the pure 2D lead?iodide perovskite family, to the best of our knowledge. More importantly, this pure 2D (3-APN)2PbI4 perovskite based PSC demonstrates excellent stability against humidity. This work demonstrates that there is great potential to realize efficient and stable pure 2D perovskite based PSCs through the wise design of organic cations.
关键词： crystal orientation,3-aminopropionitrile,pure 2D,energy level alignment,perovskite solar cells
更新于2025-09-23 15:21:01
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Shallow and Deep Trap States Passivation for Low-Temperature Processed Perovskite Solar Cells
摘要： While perovskite solar cells (PSCs) have emerged as promising low-cost solar power generators, most reported high-performance PSCs employ electron transport layers (ETLs, mainly TiO2) treated at high temperatures (≥450 °C), which may eventually hinder the development of flexible PSCs. Meanwhile, the development of low-temperature processed PSCs (L-PSCs) possessing performance levels comparable to that of high-temperature processed PSCs has actively been reported. In this study, L-PSCs with improved long-term stability and negligible hysteresis were developed through the effective passivation of shallow and deep traps in organic-inorganic hybrid perovskite (OIHP) crystals and at the ETL/OIHP interface. L-PSCs with alkaline chloride modification achieved state-of-the-art performance among reported L-PSCs (power conversion efficiency (PCE) = 22.6%) with a long-term shelf life. The origin of long-term stability and the efficient passivation of deep traps was revealed by monitoring the trap-state distribution. Moreover, the high PCE of a large-area device (21.3%, 1.12 cm2) were also demonstrated, confirming the uniformity of the modification.
关键词： trap states passivation,low-temperature processed,alkaline chloride modification,perovskite solar cells,long-term stability
更新于2025-09-23 15:21:01
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Vertically aligned 2D/3D Pb-Sn perovskites with enhanced charge extraction and suppressed phase segregation for efficient printable solar cells
摘要： The concept of mixed 2D/3D heterostructures has emerged as an effective method in improving the stability of lead halide perovskite solar cells (PSCs), which is, however, rarely reported in lead-tin (Pb-Sn) mixed perovskite devices. Here, we report a scalable process for depositing mixed 2D/3D Pb-Sn perovskite solar cells that deliver remarkably enhanced efficiency and stability compared to their 3D counterparts. The incorporation of a small amount (3.75%) of an organic cation 2-(4-fluorophenyl)ethyl ammonium iodide (FPEAI) induces the growth of highly orientated Pb-Sn perovskite crystals perpendicularly aligned to the substrate. Moreover, for the first time, phase segregation is observed in pristine 3D Pb-Sn perovskite, which is suppressed due to the presence of the 2D perovskites. Accordingly, a high current density of 28.42 mA cm-2 is obtained due to markedly enhanced spectral response and charge extraction. Eventually, mixed 2D/3D Pb-Sn perovskite devices with a bandgap of 1.33 eV yield efficiencies as high as 17.51% and in parallel exhibit good stability.
关键词： 2D/3D heterostructures,charge extraction,Pb-Sn perovskite,solar cells,phase segregation
更新于2025-09-23 15:21:01
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Carbon electrode engineering for high efficiency all-inorganic perovskite solar cells
摘要： Carbon-based inorganic perovskite solar cells (PSCs) have demonstrated an excellent performance in the field of photovoltaics owing to their simple fabrication techniques, low-cost and superior stability. Despite the lower efficiency of devices with a carbon electrode compared with the conventional structure, the potential applications in large scale have attracted increasing attention. Herein, we employ a mixed carbon electrode inorganic PSC by incorporating one-dimensional structure carbon nanotubes (CNTs) and two-dimensional Ti3C2-MXene nanosheets into a commercial carbon paste. This mixed carbon electrode, which is different from the pure carbon electrode in showing a point-to-point contact, provides a network structure and multi-dimensional charge transfer path, which effectively increases the conductivity of the carbon electrode and carriers transport. A respectable power conversion efficiency of 7.09% is obtained through carbon/CNT/MXene mixed electrode in CsPbBr3-based solar cells.
关键词： inorganic perovskite solar cells,carbon nanotubes,carbon electrode,Ti3C2-MXene,photovoltaics
更新于2025-09-23 15:21:01
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Applications of atomic layer deposition and chemical vapor deposition for perovskite solar cells
摘要： Metal halide perovskite solar cells (PSCs) have rapidly evolved over the past decade to become a photovoltaic technology on the cusp of commercialization. In the process, numerous fabrication strategies have been explored with the goal of simultaneously optimizing for device efficiency, stability, and scalability. Chemical vapor deposition (CVD) and atomic layer deposition (ALD) have proven to be effective tools for the fabrication of various components of PSCs. This review article examines the application of CVD and ALD for the deposition and modification of charge transport layers, passivation layers, absorber materials, encapsulants, and electrodes. It outlines the use of these vapor deposition techniques in state-of-the-art, multi-junction solar cell devices, and also contains a discussion of the stability of metal halide perovskite materials under CVD and ALD conditions based on in-situ characterization reported in literature. This article concludes with insights into future CVD and ALD research directions that could be undertaken to further aid the deployment of PSCs in emerging solar photovoltaic markets.
关键词： absorber materials,passivation layers,encapsulants,atomic layer deposition,charge transport layers,chemical vapor deposition,perovskite solar cells,electrodes
更新于2025-09-23 15:21:01