We passivate TiO 2 surface with alkali metal fluorides and dilute HCl, enhancing perovskite device stability. The optimized device maintains 88% of its initial efficiency after 1000 hours of continuous light soaking.
Introducing a stoichiometric excess of lead iodide(PbI 2 ) in perovskite films has been demonstrated as an effective passivation strategy that can improve the power conversion efficiency(PCE) of perovskite solar cells(PSCs),However,excess PbI 2 is also known to accelerate the degradation of the perovskite layer.In this study,we show that this degradation primarily stems from the decomposition of PbI 2 at the bottom of the perovskite film which is exposed to light We further show that when using a two-step spin coating deposition procedure,the excess PbI 2 results from the decomposition of the perovskite during the annealing process rather than the presence of non-reacted PbI 2 .Finally,we demonstrate that the spatial distribution of PbI 2 within the perovskite films can be controlled in a way that mitigates the PbI 2 induced perovskite decomposition.In this manner,we produced devices exhibiting initial power conversion efficiencies over 25%,maintaining 98.6% after 1000 h of maximum power point tracking under continuous illumination.These findings offer valuable insights into achieving high performance PSCs through judicious process control using a two-step spin-coating procedure.
Hypothesis formulation is a creative process fundamental to scientific exploration, and there is an increasing interest in using generative AI to augment humans in this regard. This study explores the potential of large language models, particularly ChatGPT, to generate viable hypotheses within experimental materials science. Focusing on the subdomain of surface passivation of hybrid perovskites, our aim is to identify untested molecules capable of reducing surface recombination and thereby boost the efficiency of perovskite solar cells. By utilizing ChatGPT to brainstorm ideas and formulate new hypotheses, we identify polyallylamine (PAA) as a potential surface modifier, which is a molecule we would not have considered otherwise. Subsequent experimental investigations demonstrate PAA to indeed be effective in decreasing recombination rates and improving device efficiency. This demonstrates a potent synergy between human expertise and AI capabilities also in more intellectual and intuitive facets of the scientific process, such as hypothesis generation.
In the original version of the article, we developed a set of heuristics for comparing stability data, which was used to analyze the dataset from the Perovskite Database Project.After the initial publication, we received feedback from a reader and identified some errors in the original dataset.To ensure that those errors had no major influence on the conclusion, we checked the data carefully and rerun the analysis with the corrected data.The detailed results are listed below.1.The errors in the data we used to draw our conclusions come from the errors in the original database.Those existed when we downloaded the data from the Perovskite Database, and none of our operations (stability data extraction, statistical analysis, "data.m"file generation) changed the original data.After a careful check, we found 95 errors in the 7419 data points we used.Those are listed in the attached file, "data correction.xlsx", and are primarily concerned with the "Cell_architecture" parameter, i.e. mostly either nip or pin. 2. After correcting the errors, we rerun the analysis.The new results show negligible changes.This is what to be expected as only a small fraction of the dataset had the wrong cell_architecture label.
The buried interface between the electron transport layer (ETL) and the perovskite layer plays a crucial role in enhancing the power conversion efficiency (PCE) and stability of n–i–p type perovskite solar cells (PSCs). In this study, the interface between the chemical bath deposited (CBD) titanium oxide (TiO2) ETL and the perovskite layer using multi‐functional potassium trifluoromethyl sulfonate (SK) is modified. Structural and elemental analyses reveal that the trifluoromethyl sulfonate serves as a crosslinker between the TiO2 and the perovskite layer, thus improving the adhesion of the perovskite to the TiO2 ETL through strong bonding of the ─CF3 and ─SO3− terminal groups. Furthermore, the multi‐functional modifiers reduced interface defects and suppressed carrier recombination in the PSCs. Consequently, devices with a champion PCE of 25.22% and a fill factor (FF) close to 85% is achieved, marking the highest PCE and FF observed for PSCs based on CBD TiO2. The unencapsulated device maintained 81.3% of its initial PCE after operating for 1000 h.
Formamidinium lead triiodide (FAPbI3)-rich perovskite absorbers have emerged as the frontrunners for the development of perovskite solar cells (PSCs), but pristine FAPbI3 absorber exhibits phase instability because of external stressors during device manufacture and operation. In this work, we systematically study the function of a trace amount of phenyltrimethylammonium chloride (PTAC) additive in FAPbI3-based perovskites. The introduced PTAC have a strong electrostatic interaction with perovskite because of the coordination of electronrich benzene ring unit and under-coordinated Pb2+, which leads to the decrease of the trap density and the release of the lattice strain. Simultaneously, the increased work function of modulated film optimizes the band alignment, promoting carrier transport and reducing nonradiative recombination, thereby improving the opencircuit voltages and fill factors. Consequently, the modulated PSCs achieve a champion power conversion efficiency of 24.51%, and exhibit much better stability by retaining 90% of their initial efficiency after 1000 hours constant illumination under maximum power point tracking measurement.
The cement industry is one of the largest contributors to global CO2 emissions, which has been paid more attention to the research on converting the CO2 released by the cement production process. It is extremely challenging to decarbonize the cement industry, as most CO2 emissions result from the calcination of limestone (CaCO3) into CaO and CO2. In this work, we demonstrate an in situ electrochemical process that transforms CaCO3 into portlandite (Ca(OH)2, a key Portland cement precursor) and valuable carbonaceous products, which integrates electrochemical water splitting and CO2 reduction reaction with the chemical decomposition of CaCO3. With different metal catalyst electrodes (like Au, Ag, In, Cu, and Cu nanowires electrodes), we have achieved various valuable carbonaceous products, such as CO, formate, methane, ethylene, and ethane during the electrochemical CO2 process. Our work demonstrates a proof of concept for green and sustainable cement production.
Urbanization has brought adverse effects on the groundwater. Increased consumption of groundwater and decreased groundwater recharge has led to groundwater decline. As a new urban management strategy, sponge city construction is an effective way to increase the permeable areas, promote the utilization of rainwater resources, and recharge groundwater in the urban area. Low impact development (LID) is the primary facility employed by sponge city construction. In this study, the feasibility of sponge city construction was quantitatively evaluated based on the long-term groundwater data. Three monitoring wells were drilled and installed within the aquifer to observe the fluctuations in water levels from September 2018 to January 2020 in the pilot area. Several LID measures were applied in Xinhua Middle School and Gediao block, where the monitoring wells were also located. According to a statistical analysis of the 50 real-time measurements, the groundwater level dropped by 0.89 m, 3.87 m, and 1.08 m at # well Xinhua, # well Tianfang, and # well Gediao, respectively, over the past 17 months. The simple linear regression was used to make trend estimation and correlation analysis. The results indicated that groundwater levels of three monitoring wells all declined during the dry season. However, all the water levels responded to the continual precipitation and showed obvious increases during the wet season. The groundwater level increased by 0.62 m, 0.74 m, and 0.90 m at # well Xinhua, # well Tianfang, and # well Gediao, respectively, during the wet season. The LID could reduce the impervious surface and increase the low soil permeability by amending soil texture in situ. The correlation analysis further verified that the rainfall affected the local groundwater recharge. So more rainwater should be intercepted at the source and then added to the aquifer through infiltration. The sponge city construction-low impact development is expected to maximize the use of the limited rainwater resources, improve the urban ecological environment, and mitigate the adverse impacts of urban sprawl.
The cement industry is one of the largest contributors to global CO2 emissions, and it is extremely challenging to decarbonize the cement industry, as most CO2 emissions results from the calcination of limestone (CaCO3) into CaO and CO2. In this work, we demonstrate a novel electrochemical process that transforms CaCO3 into portlandite (Ca(OH)2, a key Portland cement precursor) and valuable carbonaceous products, which integrates electrochemical water splitting and CO2 reduction reaction with the chemical decomposition of CaCO3. With different metal catalyst electrodes, we have achieved Ca(OH)2 and various valuable carbonaceous products, such as CO, formate, methane, and ethylene. Our work revolutionizes cement production and provides a green and sustainable path toward carbon neutrality for the cement industry.
In the last decade, perovskite solar cells have witnessed great progress with a certified photoelectric conversion efficiency of 25.7%, which is comparable to single‐crystal silicon solar cells, but the stability issue still restricts commercialization. As a solution to stability improvement, inorganic hole transport materials (HTMs) are widely studied due to their excellent stability compared to traditional organic HTMs, as well as low fabrication cost and high conductivity. Herein, the intrinsic properties of widely studied inorganic p‐type materials for HTMs, their fabrication methods, and the progress that has been made with them are summarized. In addition, the cost of various inorganic HTMs is also discussed.
Slow water oxidation kinetics and poor charge transport restrict the development of efficient BiVO4 photoanodes for photoelectrochemical (PEC) water splitting. Oxygen vacancy as an effective strategy can significantly enhance charge transport and improve conductivity in semiconductor photoanodes. Herein, we obtained BiVO4 photoanodes with appropriate oxygen vacancy by treating them with hypophosphite, which significantly improved the PEC performance. The synthesized photoanode exhibits a remarkable photocurrent density of 3.37 mA/cm2 at 1.23 V vs reversible hydrogen electrode with excellent stability. Interestingly, the performance improvement mainly originates from the oxygen vacancy rather than P doping. Our study provides insights in understanding the role of oxygen vacancy in PEC water splitting and strategies for designing more efficient photoelectrodes.
During the last decade lead halide perovskites have shown great potential for photovoltaic applications. However, the stability of perovskite solar cells still restricts commercialization, and lack of properly implemented unified stability testing and disseminating standards makes it difficult to compare historical stability data for evaluating promising routes towards better device stability. Here, we propose a single indicator to describe device stability that normalizes the stability results with respect to different environmental stress conditions which enables a direct comparison of different stability results. Based on this indicator and an open dataset of heterogeneous stability data of over 7000 devices, we have conducted a statistical analysis to assess the effect of different stability improvement strategies. This provides important insights for achieving more stable perovskite solar cells and we also provide suggestions for future directions in the perovskite solar cell field based on big data utilization.
The photo-electro catalysis has emerged as efficient and sustainable degradation method for antibiotics, where metal oxide anode plays a critical role. Exploring novel preparation method for anodes catalysis to achieve larger active sites and diverse oxidants production can directly enhance the degradation performance. Therefore, in this work, a new urea precipitation method for anode formation was studied. Both novel urea precipitation Ti/SnO2-Sb anode (TSSA-U) and traditional electro-deposition Ti/SnO2-Sb anode (TSSA-E) were prepared for Norfloxacin degradation by photo-electro catalysis in saline water. A unique tubular Ti/SnO2-Sb units formatted by urea precipitation resulted in higher porosity. This led to dominating advantage for TSSA-U on photo/electrochemical activity and degradation performances by individual photo/electro catalysis, compared to TSSA-E. However, this gap of degradation performances shrank when synergistic effect of photo-electro catalysis involved. The highest TOC removal ratio of 91.1% was obtained from TSSA-U under photo-electro catalysis. Besides, a novel BP-neural-network-physical modeling (BP-ANN-P) was developed for analysis. According to this modeling, both direct (adsorptiondegradation, radiation, etc.) and indirect (mainly .Cl) routes contributed significantly in degradation work by TSSA-U, where indirect route shared 41.8-90.1% of total degradation ratio. An increasing of current density (from 5 to 25 mA cm(-2)) enhanced the kinetics for both routes. Indirect route preferred pH = 3-7 with direct route enhanced by neutral condition. Moreover, indirect route also showed better adaptability with higher initial NOR loadings. Both urea precipitation and BP-ANN-P have shown their value for high performance material formation and data analysis, respectively. Notably, higher catalysis performance and better analysis connect to low energy cost, shorter running time and more efficient judgement and selection, which meets the requirement of cleaner production and environmental sustainability. (c) 2020 Elsevier Ltd. All rights reserved.
Inorganic cesium lead halide perovskite solar cells are promising candidates for next‐generation photovoltaic applications. However, their phase instability and relatively low efficiency hinder their commercialization. Herein, hydrophobic organic ammonium halides (Cl, Br, and I) are rationally used for the modification of inorganic CsPb(I 0.75 Br 0.25 ) 3 perovskite solar cells. Benefiting from their passivation effects and hydrophobic long alkyl chain, the modified devices exhibit enhanced efficiency and stability. Among them, the hexadecyltrimethylammonium chloride (CTAC)‐modified device shows the best performance with a power conversion efficiency (PCE) of 18.05%. Furthermore, a gradient triple anion inorganic perovskite CsPb(I 0.75 Br 0.25 ) 3− x Cl x layer is formed in situ during the CTAC modification, which demonstrates better phase stability than CsPb(I 0.75 Br 0.25 ) 3 . As a result, the modified device also shows excellent stability, maintaining 94% of the initial efficiency after 35 days in N 2 atmosphere.
Cesium lead iodide (CsPbl 3 ) is a promising photo-absorber for perovskite photovoltaics due to its high thermal stability and relatively small bandgap. However, there are many defects in solution processed polycrystalline CsPbl 3 films especially at the grain boundaries (GBs), which limit the power conversion efficiency (PCE) of CsPbl 3 solar cells. in this work, we introduced CsPbBr 3 quantum dots (QDs) on top of the CsPbl 3 film to passivate the defects. As CsPbBr 3 QDs have a small size and a similar crystal structure as the CsPbl 3 , they are excellent modifiers to fill in the GBs and heal the defects. Moreover, we find there is an anion exchange reaction between the CsPbBr 3 QDs and CsPbl 3 films, which is evidenced by photoluminescence spectra and grazing incidence X-ray diffraction patterns. The QDs treated films show enhanced carrier lifetime and reduced defect density. Additionally, the ligands on CsPbBr 3 QDs increase the hydrophobicity of the films. As a result, the QDs treated CsPbl 3 solar cells prepared at high temperature obtain PCEs exceeding 16% with high stability.
The commercialization of perovskite solar cells is mainly limited by their operational stability. Interlayer modification by thin interface materials between the perovskite and the charge transport layers is one of the most effective methods to promote the efficiency and stability of perovskite devices. However, the commonly used interlayer materials do not meet all the demands, including good film quality, excellent stability, and passivation capability without interfering with the charge transport. In this work, we propose a new material, water stable haloplumbate [TBA]PbI3 for interfacial modification, which is formed on the perovskite surface in-situ by tetra-butylammonium iodide (TBAI) treatment. Benefiting from its passivation effect and robustness, the modified devices result in a power conversion efficiency of 22.90% with excellent environmental and operational stability.
Excess lead iodide (PbI2 ), as a defect passivation material in perovskite films, contributes to the longer carrier lifetime and reduced halide vacancies for high-efficiency perovskite solar cells. However, the random distribution of excess PbI2 also leads to accelerated degradation of the perovskite layer. Inspired by nanocrystal synthesis, here, a universal ligand-modulation technology is developed to modulate the shape and distribution of excess PbI2 in perovskite films. By adding certain ligands, perovskite films with vertically distributed PbI2 nanosheets between the grain boundaries are successfully achieved, which reduces the nonradiative recombination and trap density of the perovskite layer. Thus, the power conversion efficiency of the modulated device increases from 20% to 22% compared to the control device. In addition, benefiting from the vertical distribution of excess PbI2 and the hydrophobic nature of the surface ligands, the modulated devices exhibit much longer stability, retaining 72% of their initial efficiency after 360 h constant illumination under maximum power point tracking measurement.
A series of solid electrolyte cells with La0.8Sr0.2MnO3 (LSM)-Ce0.8Sm0.2O1.9 (SDC) composite cathodes was fabricated for the electrochemical decomposition of nitric oxide (NO). The LSM and SDC powders were synthesized by a combined EDTA-citrate method. Thermogravimetry with differential scanning calorimetry, X-ray diffraction analysis, scanning and transmission electron microscope with electron diffraction were performed to characterize the synthesized powders. The NO conversions and power consumptions of the solid electrolyte cells with the cathodes sintered at 900-1200 degrees C were evaluated. The electrochemical properties, microstructures, and crystalline phases of the cathodes were further studied by electrochemical impedance spectrum, scanning electron microscope and X-ray diffraction, respectively. The NO conversions and electrochemical performances of the cells at different operating temperature were also investigated. It was concluded that the LSM and SDC powders calcined at 900 degrees C both showed good crystal structures with high purity. The cell with the cathode sintered at 1100 degrees C had the highest NO conversion of 65.4% and the lowest power consumption of 0.2024 W under 80 mA applied current. The total polarization resistances of the cells with the cathodes sintered at 900-1200 degrees C were 63.32, 41.75, 38.11 and 97.57 Omega cm(2) in 800 ppm NO, respectively. The cathode sintered at 900 degrees C had an incompact structure and connected with the electrolyte loosely, thereby impeding the NO adsorption on the cathode surface and the transfer of O2- from three phase boundary (TPB) to electrolyte. The excess sintering temperature of 1200 degrees C resulted in a dense structure of cathode and La2Zr2O7 formation at the interface between the cathode and electrolyte, thereby leading to a poor NO decomposition performance. This study also found that the NO conversion increased with the rise of operating temperature and 600 degrees C was not suitable for operation because of the electrode degradation caused by the overvoltage. (C) 2018 Elsevier B.V. All rights reserved.