Dual-Stage Reduction Strategy of Tin Perovskite Enables High Performance Photovoltaics.

The rapid oxidation of Sn2+ in tin-based perovskite solar cells (TPSCs) restricts their efficiency and stability have been main bottleneck towards further development. This study developed a novel strategy which utilizes thiosulfate ions (S2O32-) in the precursor solution to enable a dual-stage reduction process. In the solution stage, thiosulfate acted as an efficacious reducing agent to reduce Sn4+ to Sn2+, meanwhile, its oxidation products were able to reduce I2 to I- during the film stage. This dual reduction ability effectively inhibited the oxidation of Sn2+ and passivated defects, further promising an excellent stability of the perovskite devices. As a result, thiosulfate-incorporated devices achieved a high efficiency of 14.78% with open-circuit voltage reaching 0.96 V. The stability of the optimized devices achieved a remarkable improvement, maintaining 90% of their initial efficiencies after 628 hours at maximum-power-point (MPP). The findings provid research insights and experimental data support for the sustained dynamic reduction in TPSCs.

Bilateral Chemical Linking at NiOx Buried Interface Enables Efficient and Stable Inverted Perovskite Solar Cells and Modules.

Inverted NiOx-based perovskite solar cells (PSCs) exhibit considerable potential because of their low-temperature processing and outstanding excellent stability, while is challenged by the carriers transfer at buried interface owing to the inherent low carrier mobility and abundant surface defects that directly deteriorates the overall device fill factor. Present work demonstrates a chemical linker with the capability of simultaneously grasping NiOx and perovskite crystals by forming a Ni-S-Pb bridge at buried interface to significantly boost the carriers transfer, based on a rationally selected molecule of 1,3-dimethyl-benzoimidazol-2-thione (NCS). The constructed buried interface not only reduces the pinholes and needle-like residual PbI2 at the buried interface, but also deepens the work function and valence band maximum positions of NiOx, resulting in a smaller VBM offset between NiOx and perovskite film. Consequently, the modulated PSCs achieved a high fill factor up to 86.24 %, which is as far as we know the highest value in records of NiOx-based inverted PSCs. The NCS custom-tailored PSCs and minimodules (active area of 18 cm2) exhibited a champion efficiency of 25.05 % and 21.16 %, respectively. The unencapsulated devices remains over 90 % of their initial efficiency at maximum power point under continuous illumination for 1700 hours.

Characterizing Spatial and Energetic Distributions of Trap States Toward Highly Efficient Perovskite Photovoltaics.

Due to their greater opt electric performance, perovskite photovoltaics (PVs) present huge potential to be commercialized. Perovskite PV's high theoretical efficiency expands the available development area. The passivation of defects in perovskite films is crucial for approaching the theoretical limit. In addition to creating efficient passivation techniques, it is essential to direct the passivation approach by getting precise and real-time information on the trap states through measurements. Therefore, it is necessary to establish quantitative characterization methods for the trap states in energy and 3D spaces. The authors cover the characterization of the spatial and energy distributions of trap states in this article with an eye toward high-efficiency perovskite photovoltaics. After going over the strategies that have been created for characterizing and evaluating trap states, the authors will concentrate on how to direct the creative development of characterization techniques for trap states assessment and highlight the opportunities and challenges of future development. The 3D space and energy distribution mappings of trap states are anticipated to be realized. The review will give key guiding importance for further approaching the theoretical efficiency of perovskite photovoltaics, offering some future research direction and technological assistance for the development of appropriate targeted passivation technologies.

Managing Excess Lead Iodide with Functionalized Oxo-Graphene Nanosheets for Stable Perovskite Solar Cells.

Stability issues could prevent lead halide perovskite solar cells (PSCs) from commercialization despite it having a comparable power conversion efficiency (PCE) to silicon solar cells. Overcoming drawbacks affecting their long-term stability is gaining incremental importance. Excess lead iodide (PbI2 ) causes perovskite degradation, although it aids in crystal growth and defect passivation. Herein, we synthesized functionalized oxo-graphene nanosheets (Dec-oxoG NSs) to effectively manage the excess PbI2 . Dec-oxoG NSs provide anchoring sites to bind the excess PbI2 and passivate perovskite grain boundaries, thereby reducing charge recombination loss and significantly boosting the extraction of free electrons. The inclusion of Dec-oxoG NSs leads to a PCE of 23.7 % in inverted (p-i-n) PSCs. The devices retain 93.8 % of their initial efficiency after 1,000 hours of tracking at maximum power points under continuous one-sun illumination and exhibit high stability under thermal and ambient conditions.

Visualizing the Surface Photocurrent Distribution in Perovskite Photovoltaics.

Defect states play an important role in the photovoltaic performance of metal halide perovskites. Particularly, the passivation of surface defects has made great contributions to high-performance perovskite photovoltaics. This highlights the importance of understanding the surface defects from a fundamental level by developing more accurate and operando characterization techniques. Herein, a strategy to enable the surface carriers and photocurrent distributions on perovskite films to be visualized in the horizontal direction is put forward. The visual image of photocurrent distribution is realized by combining the static local distribution of carriers provided by scanning near-field optical microscopy with the dynamic transporting of carriers achieved via a scanning photocurrent measurement system. Taking a surface passivated molecule as an example, a comprehensive defect scene including static and dynamic as well as local and entire conditions is obtained using this strategy. The comprehensive analysis of the trap states in perovskite films is pioneered vertically and horizontally, which will powerfully promote the deep understanding of defect mechanisms and carrier behavior for the goal of fabricating high-performance perovskite optoelectronic devices.

Perovskite Photovoltaics for Artificial Light Harvesting.

Perovskites have encountered a growing interest as light-absorbing materials for harvesting and recycling ambient light. This interest comes from the distinct and impressive intrinsic properties of these materials and is necessitated by the need for reliable and sustainable power supplies for wearable and portable internet of things (IoT) applications. Perovskite artificial light cells (PALCs; i. e., indoor perovskite photovoltaics) have been intensively explored, and thus their device performance has been rapidly augmented. In this review, we summarize and consolidate the research outputs of PALCs by focusing on the tuning of photo-absorber and interlayer materials for efficient harvest and collection of artificial light sources. We also emphasize various challenges and possible future research directions that should be addressed for realizing a large market uptake of PALCs.

Solubility of Hybrid Halide Perovskites in DMF and DMSO.

Solution methods remain the most popular means for the fabrication of hybrid halide perovskites. However, the solubility of hybrid perovskites has not yet been quantitively investigated. In this study, we present accurate solubility data for MAPbI3, FAPbI3, MAPbBr3 and FAPbBr3 in the two most widely used solvents, DMF and DMSO, and demonstrate huge differences in the solubility behavior depending on the solution compositions. By analyzing the donor numbers of the solvents and halide anions, we rationalize the differences in the solubility behavior of hybrid perovskites with various compositions, in order to take a step forward in the search for better processing conditions of hybrid perovskites for solar cells and optoelectronics.

Stabilization of the Metastable Lead Iodide Perovskite Phase via Surface Functionalization.

Metastable structural polymorphs can have superior properties and applications to their thermodynamically stable phases, but the rational synthesis of metastable phases is a challenge. Here, a new strategy for stabilizing metastable phases using surface functionalization is demonstrated using the example of formamidinium lead iodide (FAPbI3) perovskite, which is metastable at room temperature (RT) but holds great promises in solar and light-emitting applications. We show that, through surface ligand functionalization during direct solution growth at RT, pure FAPbI3 in the cubic perovskite phase can be stabilized in nanostructures and thin films at RT without cation or anion alloying. Surface characterizations reveal that long-chain alkyl or aromatic ammonium (LA) cations bind to the surface of perovskite structure. Calculations show that such functionalization reduces the surface energy and plays a dominant role in stabilizing the metastable perovskite phase. Excellent photophysics and optically pumped lasing from the stabilized single-crystal FAPbI3 nanoplates with low thresholds were demonstrated. High-performance solar cells can be fabricated with such directly synthesized stabilized phase-pure FAPbI3 with a lower bandgap. Our results offer new insights on the surface chemistry of perovskite materials and provide a new strategy for stabilizing metastable perovskites and metastable polymorphs of solid materials in general.

Controlling Nucleation and Growth of Metal Halide Perovskite Thin Films for High-Efficiency Perovskite Solar Cells.

Metal halide perovskite thin films can be crystallized via a broad range of solution-based routes. However, the quality of the final films is strongly dependent upon small changes in solution composition and processing parameters. Here, this study demonstrates that a fractional substitution of PbCl2 with PbI2 in the 3CH3 NH3 I:PbCl2 mixed-halide starting solution has a profound influence upon the ensuing thin-film crystallization. The presence of PbI2 in the precursor induces a uniform distribution of regular quadrilateral-shaped CH3 NH3 PbI3 perovskite crystals in as-cast films, which subsequently grow to form pinhole-free perovskite films with highly crystalline domains. With this new formulation of 3CH3 NH3 I:0.98PbCl2 :0.02PbI2 , this study achieves a 19.1% current-voltage measured power conversion efficiency and a 17.2% stabilized power output in regular planar heterojunction solar cells.

Facile Tailoring of Metal-Organic Frameworks for Förster Resonance Energy Transfer-Driven Enhancement in Perovskite Photovoltaics.

Förster resonance energy transfer (FRET) has demonstrated its potential to enhance the light energy utilization ratio of perovskite solar cells by interacting with metal-organic frameworks (MOFs) and perovskite layers. However, comprehensive investigations into how MOF design and synthesis impact FRET in perovskite systems are scarce. In this work, nanoscale HIAM-type Zr-MOF (HIAM-4023, HIAM-4024, and HIAM-4025) is meticulously tailored to evaluate FRET's existence and its influence on the perovskite photoactive layer. Through precise adjustments of amino groups and acceptor units in the organic linker, HIAM-MOFs are synthesized with the same topology, but distinct photoluminescence (PL) emission properties. Significant FRET is observed between HIAM-4023/HIAM-4024 and the perovskite, confirmed by spectral overlap, fluorescence lifetime decay, and calculated distances between HIAM-4023/HIAM-4024 and the perovskite. Conversely, the spectral overlap between the PL emission of HIAM-4025 and the perovskite's absorption spectrum is relatively minimal, impeding the energy transfer from HIAM-4025 to the perovskite. Therefore, the HIAM-4023/HIAM-4024-assisted perovskite devices exhibit enhanced EQE via FRET processes, whereas the HIAM-4025 demonstrates comparable EQE to the pristine. Ultimately, the HIAM-4023-assisted perovskite device achieves an enhanced power conversion efficiency (PCE) of 24.22% compared with pristine devices (PCE of 22.06%) and remarkable long-term stability under ambient conditions and continuous light illumination.

Photochemical Shield Enabling Highly Efficient Perovskite Photovoltaics.

Oxygen is difficult to be physically removed. Oxygen will be excited by light to form free radicals which further attack the lattice of perovskite. The stabilization of α-FAPbI3 against δ-FAPbI3 is the key to optimize perovskite solar cells. Herein, the simple molecule, benzaldehyde (BAH) is adopted. The photochemical shield will be established in perovskite layer. Moreover, heterogeneous nucleation induced by BAH enhances the crystallization of α-FAPbI3. Consequently, the stability of device is improved significantly. The target device maintains 95% of original power conversion efficiency after 1500 h under air conditions and light-emitting diode light. The power conversion efficiency increases from 23.21% of pristine device to 24.82% of target device.

Magnetic-biased chiral molecules enabling highly oriented photovoltaic perovskites.

The interaction between sites A, B and X with passivation molecules is restricted when the conventional passivation strategy is applied in perovskite (ABX3) photovoltaics. Fortunately, the revolving A-site presents an opportunity to strengthen this interaction by utilizing an external field. Herein, we propose a novel approach to achieving an ordered magnetic dipole moment, which is regulated by a magnetic field via the coupling effect between the chiral passivation molecule and the A-site (formamidine ion) in perovskites. This strategy can increase the molecular interaction energy by approximately four times and ensure a well-ordered molecular arrangement. The quality of the deposited perovskite film is significantly optimized with inhibited nonradiative recombination. It manages to reduce the open-circuit voltage loss of photovoltaic devices to 360 mV and increase the power conversion efficiency to 25.22%. This finding provides a new insight into the exploration of A-sites in perovskites and offers a novel route to improving the device performance of perovskite photovoltaics.

Mechanical Durability and Flexibility in Perovskite Photovoltaics: Advancements and Applications.

The remarkable progress in perovskite solar cell (PSC) technology has witnessed a remarkable leap in efficiency within the past decade. As this technology continues to mature, flexible PSCs (F-PSCs) are emerging as pivotal components for a wide array of applications, spanning from powering portable electronics and wearable devices to integrating seamlessly into electronic textiles and large-scale industrial roofing. F-PSCs characterized by their lightweight, mechanical flexibility, and adaptability for cost-effective roll-to-roll manufacturing, hold immense commercial potential. However, the persistent concerns regarding the overall stability and mechanical robustness of these devices loom large. This comprehensive review delves into recent strides made in enhancing the mechanical stability of F-PSCs. It covers a spectrum of crucial aspects, encompassing perovskite material optimization, precise crystal grain regulation, film quality enhancement, strategic interface engineering, innovational developed flexible transparent electrodes, judicious substrate selection, and the integration of various functional layers. By collating and analyzing these dedicated research endeavors, this review illuminates the current landscape of progress in addressing the challenges surrounding mechanical stability. Furthermore, it provides valuable insights into the persistent obstacles and bottlenecks that demand attention and innovative solutions in the field of F-PSCs.

Transition metals-based electrocatalysts on super-flat substrate for perovskite photovoltaic hydrogen production with 13.75% solar to hydrogen efficiency.

Harnessing the inexhaustible solar energy for water splitting is regarded one of the most promising strategies for hydrogen production. However, sluggish kinetics of oxygen evolution reaction (OER) and expensive photovoltaics have hindered commercial viability. Here, an adhesive-free electrodeposition process is developed for in-situ preparation of earth-abundant electrocatalysts on super-flat indium tin oxide (ITO) substrate. NiFe hydroxide exhibited prominent OER performance, achieving an ultra-low overpotential of 236 mV at 10 mA/cm2 in alkaline solution. With the superior OER activity, we achieved an unassisted solar water splitting by series connected perovskite solar cells (PSCs) of 2 cm2 aperture area with NiFe/ITO//Pt electrodes, yielding overall solar to hydrogen (STH) efficiency of 13.75 %. Furthermore, we upscaled the monolithic facility to utilize perovskite solar module for large-scale hydrogen production and maintained an approximate operating current of 20 mA. This creative strategy contributes to the decrease of industrial manufacturing expenses for perovskite-based photovoltaic-electrochemical (PV-EC) hydrogen production, further accelerating the conversion and utilization of carbon-free energy.

Lead Isolation and Capture in Perovskite Photovoltaics toward Eco-Friendly Commercialization.

Perovskite solar cells (PSCs) are developed rapidly in efficiency and stability in recent years, which can compete with silicon solar cells. However, an important obstacle to the commercialization of PSCs is the toxicity of lead ions (Pb2+) from water-soluble perovskites. The entry of free Pb2+ into organisms can cause severe harm to humans, such as blood lead poisoning, organ failure, etc. Therefore, this work reports a "lead isolation-capture" dual detoxification strategy with calcium disodium edetate (EDTA Na-Ca), which can inhibit lead leakage from PSCs under extreme conditions. More importantly, leaked lead exists in a nontoxic aggregation state chelated by EDTA. For the first time, in vivo experiments are conducted in mice to systematically prove that this material has a significant inhibitory effect on the toxicity of perovskites. In addition, this strategy can further enhance device performance, enabling the optimized devices to achieve an impressive power conversion efficiency (PCE) of 25.19%. This innovative strategy is a major breakthrough in the research on the prevention of lead toxicity in PSCs.

Solution-Processed Micro-Nanostructured Electron Transport Layer via Bubble-Assisted Assembly for Efficient Perovskite Photovoltaics.

Organic-inorganic halide perovskite solar cells (PSCs) have attracted significant attention in photovoltaic research, owing to their superior optoelectronic properties and cost-effective manufacturing techniques. However, the unbalanced charge carrier diffusion length in perovskite materials leads to the recombination of photogenerated electrons and holes. The inefficient charge carrier collecting process severely affects the power conversion efficiency (PCE) of the PSCs. Herein, a solution-processed SnO2 array electron transport layer with precisely tunable micro-nanostructures is fabricated via a bubble-template-assisted approach, serving as both electron transport layers and scaffolds for the perovskite layer. Due to the optimized electron transporting pathway and enlarged perovskite grain size, the PSCs achieve a PCE of 25.35% (25.07% certificated PCE).

Crystallization Control for Ambient Printed FA-Based Lead Triiodide Perovskite Solar Cells.

Upscalable printing of high-performance and stable perovskite solar cells (PSCs) is highly desired for commercialization. However, the efficiencies of printed PSCs lag behind those of their lab-scale spin-coated counterparts owing to the lack of systematic understanding and control over perovskite crystallization dynamics. Here, the controlled crystallization dynamics achieved using an additive 1-butylpyridine tetrafluoroborate (BPyBF4 ) for high-quality ambient printed α-formamidinium lead triiodide (FAPbI3 ) perovskite films are reported. Using in situ grazing-incidence wide-angle X-ray scattering and optical diagnostics, the spontaneous formation of α-FAPbI3 from precursors during printing without the involvement of  Î´-FAPbI3 is demonstrated. The addition of BPyBF4 delays the crystallization onset of α-FAPbI3 , enhances the conversion from sol-gel to perovskite, and reduces stacking defects during printing. Therefore, the altered crystallization results in fewer voids, larger grains, and less trap-induced recombination loss within printed films. The printed PSCs yield high power conversion efficiencies of 23.50% and 21.60% for a 0.09 cm-2 area device and a 5 cm × 5 cm-area module, respectively. Improved device stability is further demonstrated, i.e., approximately 94% of the initial efficiency is retained for over 2400 h under ambient conditions without encapsulation. This study provides an effective crystallization control method for the ambient printing manufacture of large-area high-performance PSCs.

Long-Chain Gemini Surfactant-Assisted Blade Coating Enables Large-Area Carbon-Based Perovskite Solar Modules with Record Performance.

Carbon-based perovskite solar cells show great potential owing to their low-cost production and superior stability in ambient air. However, scaling up to high-efficiency carbon-based solar modules hinges on reliable deposition of uniform defect-free perovskite films over large areas, which is an unsettled but urgent issue. In this work, a long-chain gemini surfactant is introduced into perovskite precursor ink to enforce self-assembly into a network structure, considerably enhancing the coverage and smoothness of the perovskite films. The long gemini surfactant plays a distinctively synergistic role in perovskite film construction, crystallization kinetics modulation and defect passivation, leading to a certified record power conversion efficiency of 15.46% with Voc of 1.13 V and Jsc of 22.92 mA cm-2 for this type of modules. Importantly, all of the functional layers of the module are printed through a simple and high-speed (300 cm min-1) blade coating strategy in ambient atmosphere. These results mark a significant step toward the commercialization of all-printable carbon-based perovskite solar modules.

Full-Dimensional Grain Boundary Stress Release for Flexible Perovskite Indoor Photovoltaics.

Perovskite photovoltaics are strong potential candidates to drive low-power off-grid electronics for indoor applications. Compared with rigid devices, flexible perovskite devices can provide a more suitable surface for indoor small electronic devices, enabling them have a broader indoor application prospect. However, the mechanical stability of flexible perovskite photovoltaics is an urgent issue solved. Herein, a kind of 3D crosslinking agent named borax is selected to carry out grain boundary penetration treatment on perovskite film to realize full-dimensional stress release. This strategy improves the mechanical and phase stabilities of perovskite films subjected to external forces or large temperature changes. The fabricated perovskite photovoltaics deliver a champion power conversion efficiency (PCE) of 21.63% under AM 1.5G illumination, which is the highest one to date. The merit of low trap states under weak light makes the devices present a superior indoor PCE of 31.85% under 1062 lux (LED, 2956 K), which is currently the best flexible perovskite indoor photovoltaic device. This work provides a full-dimensional grain boundary stress release strategy for highly stable flexible perovskite indoor photovoltaics.

Deleterious Effects of Halides and Solvents used in Electronic Device Fabrication on the Integrity of Copper Iodide Thin-Films.

Copper iodide (CuI) is a promising material for use as hole-transport layers in electronic devices due to their solution processability and efficient hole conductivity. CuI has a rich chemistry with halide salts and solvents to which it may be exposed during device fabrication. Thus, care must be taken during device fabrication when CuI is used. We present a study using CuI as a hole transport layer in a p-i-n perovskite photovoltaic architecture. We studied how each of the components present in the perovskite precursor solution impacts the integrity of CuI films using power x-ray diffraction, UV-vis spectroscopy and impedance spectroscopy. Based on these studies, we show that DMSO, mixtures of γ-butyrolactone:DMSO (v/v 7 : 3) and DMF:DMSO (v/v 8 : 2), and iodide ions can dissolve the CuI layer. We also how that by coating a layer of copper(II) acetate and utilizing the known Cu(II)/Cu(I) redox chemistry with iodide ions, we can preserve CuI in the presence of halide salts and solvents.