Abstract:The moisture instability of organic−inorganic hybrid perovskite solar cells has been a major obstacle to the commercialization, calling for mechanistic understanding of the degradation process, which has been under debate. Here we present a surprising discovery that the degradation is actually reversible, via in situ observation of X-ray diffraction, supported by FTIR and SEM. To isolate the hydrogen bond effect, water was replaced by methanol during the in situ experiment, revealing the decomposition to be in… Show more
“…Despite many mechanisms having been reported before [17][18][19][20][21][22], they were often inconsistent and self-contradictory. Hopefully, some of the conflicts can be neutralized by our recently published work, where we revealed the importance of hydrogen bonding for the perovskite structural stability and discovered the true cause of the irreversible degradation [10]. However, there remains some other substance detected during the synthesis of the CH 3 NH 3 PbI 3 thin film, which has yet to be identified by the perovskite solar cell community, despite the fact that a similar phenomenon was also reported before elsewhere [23,24].…”
Section: Introductionmentioning
confidence: 53%
“…While such record performance seems to be inspiring for renewable energy development, the device lifetime, especially under moisture environment, remains at a low level, which prevents its commercialization. The devices usually degrade within a day unless an extra encapsulation layer is adopted [5][6][7], and even with the encapsulation layer the longest lifetime reported is still less than 4000 hours, which is far from enough for commercialization [8][9][10].…”
Extra peaks have constantly been observed in the X-ray diffraction measurement for the CH3NH3PbI3 film. Such mysteries have now been uncovered in this paper, in which powder X-ray diffraction, in situ X-ray diffraction, and scanning electron microscopy measurements were conducted, and these peaks were attributed to the ethylammonium lead iodide (CH3CH2NH3PbI3/EAPbI3). It was found that the formation of EAPbI3 was triggered by the breakdown of N, N-dimethylformamide (DMF), which was adopted as the solvent in the preparation of the precursor solutions. EAPbI3 was generated by the organic cation exchange reaction in the subsequent annealing process. A simple solution for this problem is proposed in this paper as well, which would hopefully help the community to eradicate this impurity.
“…Despite many mechanisms having been reported before [17][18][19][20][21][22], they were often inconsistent and self-contradictory. Hopefully, some of the conflicts can be neutralized by our recently published work, where we revealed the importance of hydrogen bonding for the perovskite structural stability and discovered the true cause of the irreversible degradation [10]. However, there remains some other substance detected during the synthesis of the CH 3 NH 3 PbI 3 thin film, which has yet to be identified by the perovskite solar cell community, despite the fact that a similar phenomenon was also reported before elsewhere [23,24].…”
Section: Introductionmentioning
confidence: 53%
“…While such record performance seems to be inspiring for renewable energy development, the device lifetime, especially under moisture environment, remains at a low level, which prevents its commercialization. The devices usually degrade within a day unless an extra encapsulation layer is adopted [5][6][7], and even with the encapsulation layer the longest lifetime reported is still less than 4000 hours, which is far from enough for commercialization [8][9][10].…”
Extra peaks have constantly been observed in the X-ray diffraction measurement for the CH3NH3PbI3 film. Such mysteries have now been uncovered in this paper, in which powder X-ray diffraction, in situ X-ray diffraction, and scanning electron microscopy measurements were conducted, and these peaks were attributed to the ethylammonium lead iodide (CH3CH2NH3PbI3/EAPbI3). It was found that the formation of EAPbI3 was triggered by the breakdown of N, N-dimethylformamide (DMF), which was adopted as the solvent in the preparation of the precursor solutions. EAPbI3 was generated by the organic cation exchange reaction in the subsequent annealing process. A simple solution for this problem is proposed in this paper as well, which would hopefully help the community to eradicate this impurity.
“…In order to investigate the effects of perovskite modification on the device stability under external stress, we tested the effects of light soaking, thermal degradation, and moisture59–61 as shown in Figure 5d–f. The control PSC device only retains about 20% of its original PCE after 100 h illumination (at one sun, without UV filter, humidity level of 50%) and less than 20% after 100 h storage at 80 °C in nitrogen atmosphere.…”
A strategy for efficaciously regulating perovskite crystallinity is proposed by using a volatile solid glycolic acid (HOCH2COOH, GA) in an FA0.85MA0.15PbI3 (FA: HC(NH2)2; MA: CH3NH3) perovskite precursor solution that is different from the common additive approach. Accompanied with the first dimethyl sulfoxide sublimation process, the subsequent sublimation of GA before 150 °C in the FA0.85MA0.15PbI3 perovskite film can artfully regulate the perovskite crystallinity without any residual after annealing. The improved film formation upon GA modification induced by the strong interaction between GA and Pb2+ delivers a champion power conversion efficiency (PCE) as high as 21.32%. In order to investigate the role of volatility in perovskite solar cells (PSCs), nonvolatile thioglycolic acid (HSCH2COOH, TGA) with a similar structure to GA is utilized as an additive reference. Large perovskite grains are obtained by TGA modification but with obvious pinholes, which directly leads to an increased defect density accompanied by a decline in PCE. Encouragingly, the champion PCE achieved for GA‐based PSC device (21.32%) is almost 13% or 20% higher than those of the control device or TGA‐based device. In addition, GA‐modified PSCs exhibit the best stability in light‐, thermal‐, and humidity‐based tests due to the improved film formation.
“…Moreover, this peak in the latter sample is extremely strong. As the —OH group in methanol can disrupt the interaction between methylammonium cation (MA + ) and PbX 6 octahedra, [ 25 ] so the perovskite film will undergo the loss of organic composition as MA + and generate PbI 2 . However, when the concentration of CsBr increases, Cs + ions can react with perovskite film to fill the A‐site vacancy and restore the perovskite structure.…”
It is challenging to passivate defects that are buried in the depth of perovskite films; most of the reported passivation methods cannot reach the deep defects. Herein, methanol is adopted as a dual‐functional reagent to not only act as a solvent but also help the dissolved ions penetrate the depth of perovskite films. By treating the as‐prepared perovskite films with CsBr/methanol solution, Br− ions can react with the undercoordinated Pb2+, and Cs+ ions can fill in the cation vacancies. This strategy enables surface and bulk defects passivation to be achieved simultaneously. The nonradiative recombination of the double‐passivated devices is significantly suppressed and the migration of charged defects is remarkably hindered. As a result, an improved power conversion efficiency of 19.5% and an open‐circuit voltage of 1.183 V is achieved. Moreover, the passivated device can retain ≈80% of the initial efficiency after working for 500 h at maximum power point under 1‐sun illumination, whereas the pristine device reaches 80% of the initial efficiency after only 90 h. This work demonstrates that surface and bulk defects passivation is critical to improve the efficiency and long‐term operational stability of the perovskite solar cells.
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