<i>N</i>-Methyl-2-pyrrolidone as an excellent coordinative additive with a wide operating range for fabricating high-quality perovskite films

Cheng, Fangwen; Jing, Xiaojing; Chen, Ruihao; Cao, Jing; Yan, Juanzhu; Wu, Youyunqi; Huang, Xiwei; Wu, Binghui; Zheng, Nanfeng

doi:10.1039/c9qi00547a

Cited by 28 publications

(23 citation statements)

References 36 publications

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“…[ 35 ] On the other hand, PbI 2 .NMP (Figure 1g) consists of double‐chains of edge‐sharing PbI 5 O octahedra with unshared apexes stabilized by NMP coordinated with Pb atoms, similar to PbI 2 (DMSO). [ 37,38 ] In other words, the intermediate formed using NMP does not present any contribution from MA molecules differently from the DMSO intermediate. The Gutmann acceptor donor number (DN) measures the strength of the solvents as Lewis bases.…”

Section: Resultsmentioning

confidence: 99%

Revealing the Perovskite Film Formation Using the Gas Quenching Method by In Situ GIWAXS: Morphology, Properties, and Device Performance

Szostak

Sánchez

Marchezi

et al. 2020

Adv Funct Materials

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The optoelectronic properties, morphology, and consequently the performance of metal halide perovskite solar cells are directly related to the crystalline phases and intermediates formed during film preparation. The gas quenching method is compatible with large‐area deposition, but an understanding of how this method influences these properties and performance is scarce in the literature. Here, in situ grazing incidence wide angle X‐ray scattering is employed during spin coating deposition to gain insights on the formation of MAPbI3 and CsxFA1−xPb(I0.83Br0.17)3 perovskites, comparing the use of dimethyl sulfoxide (DMSO) and 2‐methyl‐n‐pyrrolidone (NMP) as coordinative solvents. Intermediates formed using DMSO depend on the perovskite composition (e.g., Cs content), while for NMP the same intermediate [PbI2(NMP)] is formed independently on the composition. For MAPbI3 and CsxFA1−xPb(I0.83Br0.17)3 with a small amount of Cs (10% and 20%), the best efficiencies are achieved using NMP, while the use of DMSO is preferred for higher (30% and 40%) amount of Cs. The inhibition of the 2H/4H hexagonal phase when using NMP is crucial for the final performance. These findings provide a deep understanding about the formation mechanism in multication perovskites and assist the community to choose the best solvent for the desired perovskite composition aiming to perovskite‐on‐silicon tandem solar cells.

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Section: Resultsmentioning

confidence: 99%

Revealing the Perovskite Film Formation Using the Gas Quenching Method by In Situ GIWAXS: Morphology, Properties, and Device Performance

Szostak

Sánchez

Marchezi

et al. 2020

Adv Funct Materials

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“…These two φ phases are related to the formation of PbI 2 complexes involving the solvent molecules, PbI 2 ─DMF and PbI 2 ─NMP. [30,32,37] Interestingly, these diffraction peaks gradually disappear with the addition of MACl into the precursor solution. Such a phenomenon was noticed by Li et al, [38] who identified an identical trend, for double-cation MA/FA deposition, by spin coating.…”

Section: Crystallization Differences Between Vacuum Extraction and Antisolvent Methodsmentioning

confidence: 99%

“…[26] In this work, we focused on a double-cation (FA 0.83 Cs 0.17 )/ double-anion (I 0.83 Br 0.17 ) 3 perovskite composition better suited to tandem applications due to its high-bandgap value (E g ¼ 1.64 eV) compared with MAPbI 3 counterpart. Engineering of the ink formulation by the introduction of methylammonium chloride (MACl), [27][28][29] together with N-Methyl-2-pyrrolidone (NMP), [30][31][32] is herein studied, these additives being known to influence the crystal growth. Based on a holistic optimization of the triptych constituted by ink formulation, the slot-die deposition parameters, and the vacuum drying process, we achieved pinhole-free deposition on a large area (5 Â 10 cm 2 ) of Cs 0.17 FA 0.83 Pb(I 0.83 Br 0.17 ) 3 perovskite films.…”

Section: Introductionmentioning

confidence: 99%

One‐Step Slot‐Die Coating Deposition of Wide‐Bandgap Perovskite Absorber for Highly Efficient Solar Cells

et al. 2021

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Slot‐die coating is a promising technique paving the way for large‐area perovskite deposition and commercially relevant solar device fabrication with sharp control over the thickness and material composition. However, before transferring perovskite solar cells technology to commercial applications, it is required to develop ink formulations, guaranteeing high homogeneity over a wide surface and leading to large, defect‐free, and well‐crystallized perovskite grains to maximize the device performances. A one‐step slot‐die deposition route, combining ink tailoring and vacuum aspiration solvent extraction, affording the deposition of a high‐bandgap multication perovskite, is reported. One important key is the introduction of methylammonium chloride in the ink formulation, which substantially enhances the film quality over a large area. Although the efficacy of antisolvent dripping is demonstrated on a small area, it is not compatible with larger areas. This work compares the latter with a vacuum quench protocol, allowing efficient extraction of the solvents. Considering both ink formulation engineering and vacuum solvent extraction, a stabilized power conversion efficiency of up to 17.5% is reached. This constitutes, to the best of our knowledge, the highest reported value for a high‐bandgap absorber deposited by slot‐die coating. Moreover, stability over 180 h under maximum power point conditions is herein demonstrated.

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“…In an investigation, Zhang and co-workers demonstrated that NMP as a solvent additive (when added in DMF) resulted in a high quality of perovskite film due to the Lewis acid-base reaction with Pb atom. The study revealed that intermediates obtained with different PbI 2 /NMP ratios are of the same kind, because of which, the solar cell performance and stability do not depend on the NMP ratio in the precursor [51]. Following the idea of the Lewis acid-base interaction, KIM and co-workers explored pyrrolidone-based solvent additives and compared with commonly used DMF-based precursor [52].…”

Section: N Donor Atom-based Additives 211 Amine Additivesmentioning

confidence: 99%

The Progress of Additive Engineering for CH3NH3PbI3 Photo-Active Layer in the Context of Perovskite Solar Cells

Mangrulkar

Stevenson

2021

Crystals

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Methylammonium lead triiodide (CH3NH3PbI3/MAPbI3) is the most intensively explored perovskite light-absorbing material for hybrid organic–inorganic perovskite photovoltaics due to its unique optoelectronic properties and advantages. This includes tunable bandgap, a higher absorption coefficient than conventional materials used in photovoltaics, ease of manufacturing due to solution processability, and low fabrication costs. In addition, the MAPbI3 absorber layer provides one of the highest open-circuit voltages (Voc), low Voc loss/deficit, and low exciton binding energy, resulting in better charge transport with decent charge carrier mobilities and long diffusion lengths of charge carriers, making it a suitable candidate for photovoltaic applications. Unfortunately, MAPbI3 suffers from poor photochemical stability, which is the main problem to commercialize MAPbI3-based perovskite solar cells (PSCs). However, researchers frequently adopt additive engineering to overcome the issue of poor stability. Therefore, in this review, we have classified additives as organic and inorganic additives. Organic additives are subclassified based on functional groups associated with N/O/S donor atoms; whereas, inorganic additives are subcategorized as metals and non-metal halide salts. Further, we discussed their role and mechanism in terms of improving the performance and stability of MAPbI3-based PSCs. In addition, we scrutinized the additive influence on the morphology and optoelectronic properties to gain a deeper understanding of the crosslinking mechanism into the MAPbI3 framework. Our review aims to help the research community, by providing a glance of the advancement in additive engineering for the MAPbI3 light-absorbing layer, so that new additives can be designed and experimented with to overcome stability challenges. This, in turn, might pave the way for wide scale commercial use.

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N-Methyl-2-pyrrolidone as an excellent coordinative additive with a wide operating range for fabricating high-quality perovskite films

Abstract: N-Methyl-2-pyrrolidone (NMP), forming only one PbI2·NMP complex, is demonstrated as an excellent coordinative solvent for the fabrication of high-quality perovskite thin films.

Cited by 28 publications

References 36 publications

Revealing the Perovskite Film Formation Using the Gas Quenching Method by In Situ GIWAXS: Morphology, Properties, and Device Performance

Revealing the Perovskite Film Formation Using the Gas Quenching Method by In Situ GIWAXS: Morphology, Properties, and Device Performance

One‐Step Slot‐Die Coating Deposition of Wide‐Bandgap Perovskite Absorber for Highly Efficient Solar Cells

The Progress of Additive Engineering for CH3NH3PbI3 Photo-Active Layer in the Context of Perovskite Solar Cells

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