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1.
Stability has become the main obstacle for the commercialization of perovskite solar cells (PSCs) despite the impressive power conversion efficiency (PCE). Poor crystallization and ion migration of perovskite are the major origins of its degradation under working condition. Here, high‐performance PSCs incorporated with pyridine‐2‐carboxylic lead salt (PbPyA2) are fabricated. The pyridine and carboxyl groups on PbPyA2 can not only control crystallization but also passivate grain boundaries (GBs), which result in the high‐quality perovskite film with larger grains and fewer defects. In addition, the strong interaction among the hydrophobic PbPyA2 molecules and perovskite GBs acts as barriers to ion migration and component volatilization when exposed to external stresses. Consequently, superior optoelectronic perovskite films with improved thermal and moisture stability are obtained. The resulting device shows a champion efficiency of 19.96% with negligible hysteresis. Furthermore, thermal (90 °C) and moisture (RH 40–60%) stability are improved threefold, maintaining 80% of initial efficiency after aging for 480 h. More importantly, the doped device exhibits extraordinary improvement of operational stability and remains 93% of initial efficiency under maximum power point (MPP) tracking for 540 h.  相似文献   

2.
Organic–inorganic halide perovskite solar cells (PSCs) have emerged as attractive alternatives to conventional solar cells. It is still a challenge to obtain PSCs with good thermal stability and high permanence, especially at extreme outdoor temperatures. This work systematically studies the effects of Bi3+ modification on structural, electrical, and optical properties of perovskite films (FA0.83MA0.17Pb(I0.83Br0.17)3) and the performance of corresponding PSCs. The results indicate that Bi3+ modified PSCs can achieve better thermal stability, photovoltaic response, and reproducibility compared with control cells due to the decreased grain boundaries, enhanced crystallization, and improved electron extraction from perovskite film. As a result, the modified PSC exhibits an optimized power conversion efficiency (PCE) of 19.4% compared with 18.3% for the optimized control device, accompanied by better thermoresistant ability under 100–180 °C and enhanced long‐term stability. The degradation rate of the modified device is reduced by an order of magnitude due to effective structural defect modification in perovskite photoactive layer. It could maintain more than two months at 60 °C. These results shed light on the origin of crystallization and thermal stability of perovskite films, and provide an approach to solve thermal stability issue of PSCs.  相似文献   

3.
In addition to a good perovskite light absorbing layer, the hole and electron transport layers play a crucial role in achieving high‐efficiency perovskite solar cells. Here, a simple, one‐step, solution‐based method is introduced for fabricating high quality indium‐doped titanium oxide electron transport layers. It is shown that indium‐doping improves both the conductivity of the transport layer and the band alignment at the ETL/perovskite interface compared to pure TiO2, boosting the fill‐factor and voltage of perovskite cells. Using the optimized transport layers, a high steady‐state efficiency of 17.9% for CH3NH3PbI3‐based cells and 19.3% for Cs0.05(MA0.17FA0.83)0.95Pb(I0.83Br0.17)3‐based cells is demonstrated, corresponding to absolute efficiency gains of 4.4% and 1.2% respectively compared to TiO2‐based control cells. In addition, a steady‐state efficiency of 16.6% for a semi‐transparent cell is reported and it is used to achieve a four‐terminal perovskite‐silicon tandem cell with a steady‐state efficiency of 24.5%.  相似文献   

4.
Remarkable power conversion efficiencies (PCE) of metal–halide perovskite solar cells (PSCs) are overshadowed by concerns about their ultimate stability, which is arguably the prime obstacle to commercialization of this promising technology. Herein, the problem is addressed by introducing ethane‐1,2‐diammonium (+NH3(CH2)2NH3+, EDA2+) cations into the methyl ammonium (CH3NH3+, MA+) lead iodide perovskite, which enables, inter alia, systematic tuning of the morphology, electronic structure, light absorption, and photoluminescence properties of the perovskite films. Incorporation of <5 mol% EDA2+ induces strain in the perovskite crystal structure with no new phase formed. With 0.8 mol% EDA2+, PCE of the MAPbI3‐based PSCs (aperture of 0.16 cm2) improves from 16.7% ± 0.6% to 17.9% ± 0.4% under 1 sun irradiation, and fabrication of larger area devices (aperture 1.04 cm2) with a certified PCE of 15.2% ± 0.5% is demonstrated. Most importantly, EDA2+/MA+‐based solar cells retain 75% of the initial performance after 72 h of continuous operation at 50% relative humidity and 50 °C under 1 sun illumination, whereas the MAPbI3 devices degrade by approximately 90% within only 15 h. This substantial improvement in stability is attributed to the steric and coulombic interactions of embedded EDA2+ in the perovskite structure.  相似文献   

5.
Interfacial engineering, grain boundary, and surface passivation in organic–inorganic hybrid perovskite solar cells (HyPSCs) are effective in achieving high performance and enhanced durability. Organic additives and inorganic doping are generally used to chemically modify the surface contacting charge transport layers, and/or grain boundaries so as to reduce the defect density. Here, a simple but tricky one‐step method to dope organic–inorganic hybrid perovskite with Ge for the first time is reported. Unlike Ge doping to all‐inorganic perovskites, application of GeI2 in organic–inorganic perovskite precursors is challenging due to the extremely poor solubility of GeI2 in hybrid perovskite ink, leading to failure in the formation of uniform films. However, it is found that addition of methylammonium chloride (MACl) into the precursor remarkably increases the solubility of GeI2. This MACl‐assisted Ge doping of hybrid perovskites produces high‐quality crystalline film with its surface passivated with nonvolatile GeI2 (GeO2) and the volatile MACl additive also improves the uniformity of GeO2 distribution in the perovskite films. The resulting Ge‐doped mixed cation and mixed halide perovskite films with composition FA0.83MA0.17Ge0.03Pb0.97(I0.9Br0.1)3 show superior photoluminescence lifetime, power conversion efficiency above 22%, and greater stability toward illumination and humidity, outperforming photovoltaic properties of HyPSCs prepared without the Ge doping.  相似文献   

6.
To solve critical issues related to device stability and performance of perovskite solar cells (PSCs), FA0.026MA0.974PbI3?yCly‐Cu:NiO (formamidinium methylammonium (FAMA)‐perovskite‐Cu:NiO) and Al2O3/Cu:NiO composites are developed and utilized for fabrication of highly stable and efficient PSCs through fully‐ambient‐air processes. The FAMA‐perovskite‐Cu:NiO composite crystals prepared without using any antisolvents not only improve the perovskite film quality with large‐size crystals and less grain boundaries but also tailor optical and electronic properties and suppress charge recombination with reduction of trap density. A champion device based on the composites as light absorber and Al2O3/Cu:NiO interfacial layer between electron transport layer and active layer yields power conversion efficiency (PCE) of 20.67% with VOC of 1.047 V, JSC of 24.51 mA cm?2, and fill factor of 80.54%. More importantly, such composite‐based PSCs without encapsulation show significant enhancement in long‐term air‐stability, thermal‐ and photostability with retaining 97% of PCE over 240 d under ambient conditions (25–30 °C, 45–55% humidity).  相似文献   

7.
Mixed iodide‐bromide organolead perovskites with a bandgap of 1.70–1.80 eV have great potential to boost the efficiency of current silicon solar cells by forming a perovskite‐silicon tandem structure. Yet, the stability of the perovskites under various application conditions, and in particular combined light and heat stress, is not well studied. Here, FA0.15Cs0.85Pb(I0.73Br0.27)3, with an optical bandgap of ≈1.72 eV, is used as a model system to investigate the thermal‐photostability of wide‐bandgap mixed halide perovskites. It is found that the concerted effect of heat and light can induce both phase segregation and decomposition in a pristine perovskite film. On the other hand, through a postdeposition film treatment with benzylamine (BA) molecules, the highly defective regions (e.g., film surface and grain boundaries) of the film can be well passivated, thus preventing the progression of decomposition or phase segregation in the film. Besides the stability improvement, the BA‐modified perovskite solar cells also exhibit excellent photovoltaic performance, with the champion device reaching a power conversion efficiency of 18.1%, a stabilized power output efficiency of 17.1% and an open‐circuit voltage (V oc) of 1.24 V.  相似文献   

8.
The mixed perovskite (FAPbI3)1?x (MAPbBr3)x , prepared by directly mixing different perovskite components, suffers from phase competition and a low‐crystallinity character, resulting in instability, despite the high efficiency. In this study, a dual ion exchange (DIE) method is developed by treating as‐prepared FAPbI3 with methylammonium brodide (MABr)/tert‐butanol solution. The converted perovskite thin film shows an optimized absorption edge at 800 nm after reaction time control, and the high crystallinity can be preserved after MABr incorporation. More importantly, it is found that the threshold electrical field to initiate ion migration is greatly increased in DIE perovskite thin film because excess MABr on the surface can effectively heal structural defects located on grain boundaries during the ion exchange process. It contributes to the over‐one‐month moisture stability under ≈65% room humidity (RH) and greatly enhanced light stability for the bare perovskite film. As a result of preserved high crystallinity and simultaneous grain boundary passivation, the perovskite solar cells fabricated by the DIE method demonstrate reliable reproducibility with an average power conversion efficiency (PCE) of 17% and a maximum PCE of 18.1%, with negligible hysteresis.  相似文献   

9.
Supported by the density functional theory (DFT) calculations, for the first time, a fluorinated aromatic cation, 2‐(4‐fluorophenyl)ethyl ammonium iodide (FPEAI), is introduced to grow in situ a low dimensional perovskite layer atop 3D perovskite film with excess PbI2. The resulted (p‐FC6H4C2H4NH3)2[PbI4] perovskite functions as a protective capping layer to protect the 3D perovskite from moisture. In the meantime, the thin layer facilitates charge transfer at the interfaces, thereby reducing the nonradiative recombination pathways. Laser scanning confocal microscopy unveils visually the distribution of the 2D perovskite layer on top of the 3D perovskite. When employing the 3D–2D perovskite as the absorbing layer in the photovoltaic cells, a high power conversion efficiency of 20.54% is realized. Superior device performance and moisture stability are observed with the modified perovskite over the whole stability test period.  相似文献   

10.
All‐inorganic perovskite CsPbI3 quantum dots (QDs) offer much better stability for photovoltaic applications. Unfortunately, their cell efficiencies are hindered by the low carrier transport efficiency of QD‐assembled films. In addition, agglomeration‐induced phase change of QDs poses another problem for material and device degradation. Herein, the use of µ‐graphene (µGR) to crosslink QDs to form µGR/CsPbI3 film is demonstrated. It is found that the resultant QDs film provides not only an effective channel for carrier transport, as witnessed by much improved conductivity but also significantly better stability against moisture, humidity, and high temperature stresses. The µGR/CsPbI3 based solar cell shows increased device performance. More specifically, compared to the solar cell without the µGR treatment, VOC is improved to 1.18 from 1.16 V, JSC to 13.59 from 13.17 mA cm?2, and FF to 72.6 from 68.1%, and overall power conversion efficiency to as high as 11.40 from 10.41%, a 12% increase. In addition, the instability originating from the thermal/moisture‐induced QD agglomeration is also greatly suppressed by the µGR crosslinking. The optimized device retains >98% of its initial efficiency after being stored in N2 atmosphere for one month. Importantly, under 60% humidity and 100 °C thermal stresses, the µGR/CsPbI3 devices show much better stability.  相似文献   

11.
The performance of perovskite solar cells (PSCs) relies on the synthesis method and chemical composition of the perovskite materials. So far, PSCs that have adopted two‐step sequential deposited perovskite with the state‐of‐art composition (FAPbI3)1?x(MAPbBr3)x (x < 0.05) have achieved record power conversion efficiency (PCE), while their one‐step antisolvent dripping counterparts with typical composition Cs0.05FA0.81MA0.14Pb(I0.85Br0.15)3 with more bromine have exhibited much better long‐term operational stability. Thus, halogen engineering that aims to elevate bromine content in sequential deposited perovskite film would push operational stability of PSCs toward that of antisolvent dripping deposited perovskite materials. Here, a Br‐rich seeding growth method is devised and perovskite seed solution with high bromine content is introduced into a PbI2 precursor, leading to bromine incorporation in the resulting perovskite film. Photovoltaic devices fabricated by Br‐rich seeding growth method exhibit a PCE of 21.5%, similar to 21.6% for PSCs having lower bromine content. Whereas, the operational stability of PSCs with higher bromine content is significantly enhanced, with over 80% of initial PCE retained after 500 h tracking at maximum power point under 1‐sun illumination. This work highlights the vital importance of halogen composition for the operational stability of PSCs, and introduces an effective way to incorporate bromine into mixed‐cation‐halide perovskite film via sequential deposition method.  相似文献   

12.
An electrospray deposition technique to fabricate a perovskite (CH3NH3PbI3) layer for highly stable and efficient perovskite solar cells at ambient humidity (30%–50% relative humidity) conditions is demonstrated. A detailed study is conducted to determine the effect of different electrospray parameters on the device performance and to provide a mechanistic explanation of the superior stability of the films. Due to the controlled reactivity that results in the formation of a smooth perovskite film, these cells exhibit stability exceeding 4000 h, in contrast to much lower stability of those fabricated by conventional spin coating methods. Furthermore, the perovskite film deposited by electrospray methods exhibits a self‐healing behavior when exposed to moisture. The authors hypothesize the formation of an intermediate metastable phase and smooth morphology of the film as the reason for this enhanced stability. Electrospray is a scalable technique that provides precise control over the amount of material required for deposition, reducing significant material loss that occurs in conventional solution‐based methods. Overall, this work shows that stability of perovskite solar cells can be improved by fabrication using a well controlled and optimized electrospray technique, without the use of any additives or cell encapsulants.  相似文献   

13.
Although all‐inorganic perovskite solar cells (PSCs) demonstrate high thermal stability, cesium‐lead halide perovskites with high iodine content suffer from poor stability of the black phase (α‐phase). In this study, it is demonstrated that incorporating InCl3 into the host perovskite lattice helps to inhibit the formation of yellow phase (δ‐phase) perovskite and thereby enhances the long‐term ambient stability. The enhanced stability is achieved by a strategy for the structural reconstruction of CsPbI2Br perovskite by means of In3+ and Cl? codoping, which gives rise to a significant improvement in the overall spatial symmetry with a closely packed atom arrangement due to the crystal structure transformation from orthorhombic (Pnma) to cubic (Pm‐3m). In addition, a novel thermal radiation heating method that further improves the uniformity of the perovskite thin films is presented. This approach enables the construction of all‐inorganic InCl3:CsPbI2Br PSCs with a champion power conversion efficiency of 13.74% for a small‐area device (0.09 cm2) and 11.4% for a large‐area device (1.00 cm2).  相似文献   

14.
Adding a small amount of CsI into mixed cation‐halide perovskite film via a one‐step method has been demonstrated as an excellent strategy for high‐performance perovskite solar cells (PSCs). However, the one‐step method generally relies on an antisolvent washing process, which is hard to control and not suitable for fabricating large‐area devices. Here, CsF is employed and Cs is incorporated into perovskite film via a two‐step method. It is revealed that CsF can effectively diffuse into the PbI2 seed film, and drastically enhances perovskite crystallization, leading to high‐quality Cs‐doped perovskite film with a very long photoluminescence carrier lifetime (1413 ns), remarkable light stability, thermal stability, and humidity stability. The fabricated PSCs show power conversion efficiency (PCE) of over 21%, and they are highly thermally stable: in the aging test at 60 °C for 300 h, 96% of the original PCE remains. The CsF incorporation process provides a new avenue for stable high‐performance PSCs.  相似文献   

15.
An upscalable perovskite film deposition method combining raster ultrasonic spray coating and chemical vapor deposition is reported. This method overcomes the coating size limitation of the existing stationary spray, single‐pass spray, and spin‐coating methods. In contrast with the spin‐coating method (>90% Pb waste), negligible Pb waste during PbI2 deposition makes this method more environmentally friendly. Outstanding film uniformity across the entire area of 5 cm × 5 cm is confirmed by both large‐area compatible characterization methods (electroluminescence and scattered light imaging) and local characterization methods (atomic force microscopy, scanning electron microscopy, photoluminescence mapping, UV–vis, and X‐ray diffraction measurements on multiple sample locations), resulting in low solar cell performance decrease upon increasing device area. With the FAPb(I0.85Br0.15)3 (FA = formamidinium) perovskite layer deposited by this method, champion solar modules show a power conversion efficiency of 14.7% on an active area of 12.0 cm2 and an outstanding shelf stability (only 3.6% relative power conversion efficiency decay after 3600 h aging). Under continuous operation (1 sun light illumination, maximum power point condition, dry N2 atmosphere with <5% relative humidity, no encapsulation), the devices show high light‐soaking stability corresponding to an average T80 lifetime of 535 h on the small‐area solar cells and 388 h on the solar module.  相似文献   

16.
As perovskite solar cells (PSCs) are highly efficient, demonstration of high‐performance printed devices becomes important. 2D/3D heterostructures have recently emerged as an attractive way to relieving the film inhomogeneity and instability in perovskite devices. In this work, a 2D/3D ensemble with 2D perovskites self‐assembled atop 3D methylammonium lead triiodide (MAPbI3) via a one‐step printing process is shown. A clean and flat interface is observed in the 2D/3D bilayer heterostructure for the first time. The 2D perovskite capping layer significantly suppresses nonradiative charge recombination, resulting in a marked increase in open‐circuit voltage (VOC) of the devices by up to 100 mV. An ultrahigh VOC of 1.20 V is achieved for MAPbI3 PSCs, corresponding to 91% of the Shockley–Queisser limit. Moreover, notable enhancement in light, thermal, and moisture stability is obtained as a result of the protective barrier of the 2D perovskites. These results suggest a viable approach for scalable fabrication of highly efficient perovskite solar cells with enhanced environmental stability.  相似文献   

17.
The stability of a perovskite solar cell (PSC) is enhanced significantly by applying a customized thin‐film encapsulation (TFE). The TFE is composed of a multilayer stack of organic/inorganic layers deposited by initiated chemical vapor deposition and atomic layer deposition, respectively, whose water vapor transmission rate is on the order of 10?4 g m?2 d?1 at an accelerated condition of 38 °C and 90% relative humidity (RH). The TFE is optimized, taking into consideration various aspects of thermosensitive PSCs. Lowering the process temperature is one of the most effective methods for minimizing the thermal damage to the PSC during the monolithic integration of the TFE onto PSC. The direct deposition of TFE onto a PSC causes less than 0.3% degradation (from 18.5% to 18.2%) in the power conversion efficiency, while the long‐term stability is substantially improved; the PSC retains 97% of its original efficiency after a 300 h exposure to an accelerated condition of 50 °C and 50% RH, confirming the enhanced stability of the PSC against moisture. This is the first demonstration of a TFE applied directly onto PSCs in a damage‐free manner, which will be a powerful tool for the development of highly stable PSCs with high efficiency.  相似文献   

18.
Organic–inorganic hybrid lead halide perovskites are emerging as highly promising candidates for highly efficient thin film photovoltaics due to their excellent optoelectronic properties and low‐temperature process capability. However, the long‐term stability in ambient air still is a key issue limiting their further practical applications. Herein, the enhancement of both performance and stability of perovskite solar cells is reported by employing 2D and 3D heterostructured perovskite films with unique nanoplate/nanocrystalline morphology. The 2D/3D heterostructured perovskites combine advantages of the high‐performance lead‐based perovskite 3D CH3NH3PbI3 (MAPbI3) and the air‐stable bismuth‐based quasi‐perovskite 2D MA3Bi2I9. In the 2D/3D heterostructure, the hydrophobic MA3Bi2I9 platelets vertically situate between the MAPbI3 grains, forming a lattice‐like structure to tightly enclose the 3D MAPbI3 perovskite grains. The solar cell based on the optimal 2D/3D (9.2%) heterostructured film achieves a high efficiency of 18.97%, with remarkably reduced hysteresis and significantly improved stability. The work demonstrates that construction of 2D/3D heterostructured films by hybridizing different species of perovskite materials is a feasible way to simultaneously enhance both efficiency and stability of perovskite solar cells.  相似文献   

19.
Metal halide perovskites offer a wide and tunable bandgap, making them promising candidates for top‐cell absorbers in tandem photovoltaics. In this work, the authors aim to understand the atomic layer deposition (ALD) precursor–perovskite interactions of the tin oxide ALD system and the role of organic fullerenes at the perovskite–tin oxide interface while establishing a framework for developing alternative perovskite‐compatible ALD processes in the future. It is shown, in the case of tin oxide ALD growth with tetrakis(dimethylamino)tin(IV) and water on FA0.83Cs0.17Pb(I0.83Br0.17)3 perovskite, that perovskite stability is most sensitive to metal–organic exposure at elevated temperatures with an onset near 110 °C, resulting in removal of the formamidinium cation. Transitioning from ALD to pulsed‐chemical vapor deposition tin oxide growth can minimize the degradation effects. Investigation of fullerenes at the perovskite interface shows that thin fullerene layers offer minor improvements to perovskite stability under ALD conditions, but significant enhancement in carrier extraction. Fullerene materials are undesirable due to fabrication cost and poor mechanical stability. Compositional tuning of the perovskite material can improve the fullerene‐free device performance. This method is demonstrated with a bromine‐rich perovskite phase to enable an 8.2% efficient perovskite device with all‐inorganic extraction layers.  相似文献   

20.
High temperature stable inorganic CsPbX3 (X: I, Br, or mixed halides) perovskites with their bandgap tailored by tuning the halide composition offer promising opportunities in the design of ideal top cells for high‐efficiency tandem solar cells. Unfortunately, the current high‐efficiency CsPbX3 perovskite solar cells (PSCs) are prepared in vacuum, a moisture‐free glovebox or other low‐humidity conditions due to their poor moisture stability. Herein, a new precursor system (HCOOCs, HPbI3, and HPbBr3) is developed to replace the traditional precursors (CsI, PbI2, and PbBr2) commonly used for solar cells of this type. Both the experiments and calculations reveal that a new complex (HCOOH?Cs+) is generated in this precursor system. The new complex is not only stable against aging in humid air ambient at 91% relative humidity, but also effectively slows the perovskite crystallization, making it possible to eliminate the popular antisolvent used in the perovskite CsPbI2Br film deposition. The CsPbI2Br PSCs based on the new precursor system achieve a champion efficiency of 16.14%, the highest for inorganic PSCs prepared in ambient air conditions. Meanwhile, high air stability is demonstrated for an unencapsulated CsPbI2Br PSC with 92% of the original efficiency remaining after more than 800 h aging in ambient air.  相似文献   

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