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PbI2
Materials Research Express · 2018 ·Vol. 5 ·期 6 ·066404 · IF 1.151

Synergic solventing-out crystallization with subsequent time-delay thermal annealing of PbI2 precursor in mesostructured perovskite solar cells

Fujin Jia,Yanqun Guo,Lijia Che,Zhiyong Liu,Zhigang Zeng,Chuanbing Cai

Although the two-step sequential deposition method provides an efficient route to fabricate high performance perovskite solar cells (PSSCs) with increasing reproducibility, the inefficient and incomplete conversion of PbI2 to perovskite is still quite a challenge. Following pioneering works, we found that the conversion process from PbI2 to perovskite mainly involves diffusion, infiltration, contact and reaction. In order to facilitate the conversion from PbI2 to perovskite, we demonstrate an effective method to regulate supersaturation level (the driving force to crystallization) of PbI2 by solventing-out crystallization combining with subsequent time-delay thermal annealing of PbI2 wet film. Enough voids and spaces in resulting porous PbI2 layer will be in favor of efficient diffusion, infiltration of CH3NH3I solution, and further enhance the contact and reaction between PbI2 and CH3NH3I in the whole film, leading to rapid, efficient and complete perovskite conversion with a conversion level of about 99.9%. Enhancement of light harvesting ranging from visible to near-IR region was achieved for the resultant high-quality perovskite. Upon this combined method, the fabricated mesostructured solar cells show tremendous power conversion efficiency (PCE) improvement from 3.2% to about 12.3% with less hysteresis owing to the simultaneous enhancement of short-circuit photocurrent density (Jsc), open-circuit voltage (Voc) and fill factor (FF).

CAS / MDL: 546-68-9
研究领域: 材料科学 · 能源科学
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CHEMICAL ENGINEERING JOURNAL · 2025 · IF 13.2

Additive strategy toward PbI2 film modifications for efficient perovskite solar cells fabricated in an air environment

Xiuzhen Zhang,Xiyu Wang,Xiaohuan Zhang,Yuanyuan Zhang,Yongxiu Sun,Lili Liu,Wei Yan,Ning Zhang,Changyuan Zhang,Linxing Shi

In the two-step method for perovskite film fabrication, insufficient reaction between organic ammonium salts and PbI 2 affects the active layer quality, resulting in poor power conversion efficiency (PCE). In this work, we introduce pentanamine acetic acid (PenAAc) and 5-aminovaleric acid iodine (5-AVAI) as two efficient additives to modify PbI 2 layer during perovskite films fabrication via the two-step method in an air environment. After additive modifications, the quality of both PbI 2 layers is improved: PenAAc enhances crystallinity and increases PbI 2 grain size, while 5-AVAI induces a uniform and smooth PbI 2 layer. The optimized PbI 2 films facilitate the reaction between PbI 2 and organic salts, yielding a high-quality perovskite layer with enhanced crystallinity and reduced defect density. In contrast, the macromolecule structure of 5-AVAI does not diffuse after annealing, remaining in the PbI 2 layer and exerting minimal influence on the perovskite surface. However, dissociative CH 3 COO − groups in PenAAc molecules diffuse from the PbI 2 layer to the perovskite surface during annealing, forming strong interactions between I - and Pb 2+ with CH 3 COO − groups. This further improves perovskite film quality and accelerates charge carrier extraction/transport in devices. Consequently, additive-modified perovskite solar cells achieve excellent PCEs of 24.50 % (5-AVAI) and 24.65 % (PenAAc), significantly surpassing the control device (22.84 %). Moreover, hysteresis index is reduced from 4.20 % (control) to 0.33 % (5-AVAI) and 0.08 % (PenAAc). Additionally, the modified devices also demonstrated enhanced environmental stability across humidity, light, and thermal stress conditions.

研究领域: 材料科学 · 能源技术 · 光伏器件
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Laser & Photonics Reviews · 2025 · IF 10

Complete Reaction to Remove PbI2 Residue in Photovoltaic Perovskites

Namatullah Nizamani,Xin Chen,Yan-Hui Lou,Run-Jun Jin,Kai-Li Wang,Chun-Hao Chen,Jing Chen,Yu Xia,Lei Huang,Zhao-Kui Wang

In the pursuit of high-performance FAPbI 3 -based perovskite solar cells, the two-step sequential deposition method has garnered significant attention due to its superior control over film crystallization dynamics, critical for achieving uniform, and compact perovskite layers. However, the rapid reaction between PbI 2 and FAI often results in residual PbI 2 clusters, which accelerate the degradation of perovskite solar cells (PSCs). Herein, the dual-site molecular additive 1-aminonaphthalene-6-sulfonic acid (ANSA) is introduced to achieve fast nucleation and slow crystallization, thereby enabling the formation of high-quality FAPbI 3 perovskite films. ANSA coordinates with both PbI 2 and DMSO, facilitating the formation of an improved PbI 2 (DMSO) intermediate phase, enabling a more uniform and complete conversion of PbI 2 into the perovskite phase. Additionally, the amino and sulfonic acid functional groups of ANSA contribute to the passivation of undercoordinated Pb 2+ ions, thereby perovskite films with lower trap densities and larger grain sizes are achieved. Consequently, the power conversion efficiency (PCE) increases from 23.27% in the pristine device to 25.79% for the ANSA-treated device. Furthermore, device stability is significantly improved with the modified device retaining 95% of its original PCE after 1500 h of storage.

CAS / MDL: 119-79-9
研究领域: 材料科学 · 光伏技术 · 纳米材料 · 表面化学 · 能源材料
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Nanoscale Research Letters · 2019 ·Vol. 14 ·期 1 ·1-6 · IF 3.159

The Effect of Decomposed PbI2 on Microscopic Mechanisms of Scattering in CH3NH3PbI3 Films

Shan Dan,Tong Guoqing,Cao Yunqing,Tang Mingjun,Xu Jun,Yu Linwei,Chen Kunji

Hybrid organic-inorganic perovskites (HOIPs) exhibit long electronic carrier diffusion length, high optical absorption coefficient, and impressive photovoltaic device performance. At the core of any optoelectronic device lie the charge transport properties, especially the microscopic mechanism of scattering, which must efficiently affect the device function. In this work, CH 3 NH 3 PbI 3 (MAPbI 3 ) films were fabricated by a vapor solution reaction method. Temperature-dependent Hall measurements were introduced to investigate the scattering mechanism in MAPbI 3 films. Two kinds of temperature-mobility behaviors were identified in different thermal treatment MAPbI 3 films, indicating different scattering mechanisms during the charge transport process in films. We found that the scattering mechanisms in MAPbI 3 films were mainly influenced by the decomposed PbI 2 components, which could be easily generated at the perovskite grain boundaries (GBs) by releasing the organic species after annealing at a proper temperature. The passivation effects of PbI 2 in MAPbI 3 films were investigated and further discussed with emphasis on the scattering mechanism in the charge transport process.

研究领域: 材料科学 · 凝聚态物理 · 半导体物理 · 光伏器件 · 纳米材料 · 表面与界面科学 · 功能材料 · 电子输运
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ACS Nano · 2024 · IF 15.8

Residual Stress Mitigation in Perovskite Solar Cells via Butterfly-Inspired Hierarchical PbI2 Scaffold

Gui Gao,Qinchao Zhang,Kaimo Deng,Liang Li

Residual stress in metal halide perovskite films intimately affects the photovoltaic figure of merit and longevity of perovskite solar cells. A delicate management of the crystallization kinetics is critical to the preparation of high-quality perovskite films. Only very limited methods, however, are available to regulate the residual stress of a perovskite film in a controllable manner, particularly for a perovskite film fabricated by a two-step method. Here, we demonstrate the construction of a hierarchical PbI2 scaffold inspired by Archaeoprepona demophon butterfly by combining an interlayer guided growth of porous structure and nanoimprinting. The hierarchically structured PbI2 that emulates the physical structure of the butterfly wing scale permits unimpeded permeation of organic amine salts and sufficient space for volume expansion during the crystallization process, accompanied by preferential perovskite growth of a defectless (001) crystal plane. The optimized perovskite film outperforms the control with reduced residual stress and defect density. Consequently, perovskite solar cells with a respectable power conversion efficiency reaching 23.4% (certified 23%) and an impressive open-circuit voltage of 1.184 V can be achieved. The target device can maintain 80% of initial efficiency after maximum power point tracking under illumination for 700 h. This work expands the range of engineering toward PbI2 by exploring a simultaneously tailored morphology and crystallinity and highlights the significance of a hierarchical PbI2 scaffold as an alternative choice to mitigate residual stress in a two-step processed perovskite active layer and boost the longevity of perovskite solar cells.

研究领域: 材料科学 · 太阳能 · 纳米技术 · 光伏技术
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JOURNAL OF POWER SOURCES · 2022 · IF 9.794

Suppression of PbI2 decomposition with Lewis base semicarbazide hydrochloride for photostable and efficient perovskite solar cells

Hanyu Wang,Yukun Ouyang,Wenjing Zou,Xiong Deng,Hu Luo,Xingchong Liu,Haimin Li,Ruonan Zhou,Xian Peng,Xiaoli Gong,Huxin Luo

Introducing excessive PbI 2 in perovskite is widely used to fabricate high performance perovskite solar cells (PSCs) via two-step spin coating , whereas the photoinduced decomposition of excessive PbI 2 may induce perovskite photodegradation for long-term illumination. In this work, a Lewis base semicarbazide hydrochloride (SH) is introduced in the first-step PbI 2 film, which can anchor strongly PbI 2 at the grain boundaries of perovskite, suppressing its photoinduced decomposition to Pb 0 and I 2 , and consequently enhancing the long-term photostability of PSCs. In addition, it is verified that SH can also coordinate with the uncoordinated Pb 2+ in perovskite, and thus stabilize [PbX 6 ] 4- octahedral to inhibit photoinduced ion migration. Therefore, the optimized PSC exhibits not only an improved power conversion efficiency (PCE) of 21.88%, but also an enhanced photostability with 82.8% of its initial PCE under 500 h continuous AM 1.5G illumination. This work provides a new strategy to suppress PbI 2 photoinduced decomposition and perovskite photodegradation for the realization of photostable and efficient PSCs.

研究领域: 材料科学 · 光伏技术 · 化学
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MOLECULES · 2024 ·Vol. 29 ·期 16 ·3810 · IF 4.2

The Effect of Component Defects on the Performance of Perovskite Devices and the Low-Cost Preparation of High-Purity PbI2

Boyu Dong,Yuhan Xie,Yongbing Lou

The efficiency and reproducibility of perovskite solar cells (PSCs) are significantly influenced by the purity of lead iodide (PbI2) in the raw materials used. Pb(OH)I has been identified as the primary impurity generated from PbI2in water-based synthesis. Consequently, a comprehensive investigation into the impact of Pb(OH)I impurities on film and device performance is essential. In this study, PbI2, with varying stoichiometries, was synthesized to examine the effects of different Pb(OH)I levels on perovskite device performance. The characterization results revealed that even trace amounts of Pb(OH)I impede the formation of precursor prenucleation clusters. These impurities also increase the energy barrier of the α-phase and facilitate the transition of the intermediate phase to the δ-phase. These effects result in poor perovskite film morphology and sub-optimal photovoltaic device performance. To address these issues, a cost-effective method for preparing high-stoichiometry PbI2was developed. The formation of Pb(OH)I was effectively inhibited through several strategies: adjusting solution pH and temperature, modifying material addition order, simplifying the precipitation–recrystallization process, and introducing H3PO2as an additive. These modifications enabled the one-step synthesis of high-purity PbI2. PSCs prepared using this newly synthesized high-stoichiometry PbI2demonstrated photovoltaic performance comparable to those fabricated with commercial PbI2(purity ≥ 99.999%). Our novel method offers a cost-effective alternative for synthesizing high-stoichiometry PbI2, thereby providing a viable option for the production of high-performance PSCs.

研究领域: 材料科学 · 能源技术
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ACS Sustainable Chemistry & Engineering · 2023 · IF 8.4

Hexamethylphosphoramide-Assisted Structure and Morphology Regulation of a PbI2 Film for Air-Processed Efficient Perovskite Solar Cells via a Two-Step Deposition Method

Gangyi Zeng,Guangyao Liu,Xin Li

The two-step deposited method with the advantages of high reproducibility and controllability is widely used in fabricating highly efficient perovskite solar cells (PSCs). However, it is still a challenge to fabricate air-processed PSCs through this method due to the existing techniques with glove box circumstance that are not well extended to the ambient air-condition fabrication process. Here, hexamethylphosphoramide (HMPA) used as a solvent additive is incorporated into the first-step PbI2 precursor solution, which can effectively modify the morphology and crystallinity of the PbI2 layer, thereby creating more opportunities for the infiltration of the second-step organic salt. This two-step coating leads to the full conversion from PbI2 to the perovskite crystal and large grains, reduced defects, and enhanced uniformity for the final perovskite film. Consequently, a champion efficiency of 20.84% of the HMPA-based device fabricated using this procedure is achieved. The HMPA-based device shows long-term stability of the remaining 85.7% of the initial efficiency after 1000 h of storage in an ambient air environment. This method demonstrates the great potential toward air-processed efficient PSCs.

CAS / MDL: 680-31-9
研究领域: 材料科学 · 能源技术
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Sustainable Energy & Fuels · 2017 ·Vol. 2 ·期 2 ·436-443 · IF 0

The impacts of PbI2 purity on the morphology and device performance of one-step spray-coated planar heterojunction perovskite solar cells

Jiaxu Yao,Liyan Yang,Feilong Cai,Yu Yan,Robert S. Gurney,Dan Liu,Tao Wang

We have fabricated planar heterojunction perovskite solar cells by one-step ultrasonic spray-coating of the perovskite precursor solution in air. Uniform perovskite films with high surface coverage can be prepared after optimization of the precursor solution and spray-coating parameters. We found that the purity of PbI2, although varying only from 98 to 99.9%, can significantly affect the crystallinity, grain size and boundaries of MAPbI3 films that were fabricated via one-step spray-coating, and ultimately determined the power conversion efficiency (PCE) of perovskite devices. PbI2 with a purity of 98% resulted in a low conversion of precursors to perovskites, whilst a high purity of 99.9% led to perovskites with a high crystallinity, large grain size and narrow grain boundaries. Our p–i–n type, planar heterojunction solar cell ITO/PEDOT:PSS/MAPbI3/PCBM/Ag made from MAI and 99.9% purity PbI2 achieved a maximum PCE of 12.6% without hysteresis, whereas the 98% purity PbI2-based device showed a low PCE of only 4.9% with the presence of hysteresis. However, the impacts of PbI2 purity on the device efficiency can be minimized by changing the deposition method from one-step spray-coating to a two-step spin casting approach.

研究领域: 材料科学 · 太阳能 · 光伏技术 · 纳米技术
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Nanoscale · 2016 ·Vol. 8 ·期 12 ·6600-6608 · IF 7.76

Credible evidence for the passivation effect of remnant PbI2 in CH3NH3PbI3 films in improving the performance of perovskite solar cells

Shimao Wang,Weiwei Dong,Xiaodong Fang,Qingli Zhang,Shu Zhou,Zanhong Deng,Ruhua Tao,Jingzhen Shao,Rui Xia,Chao Song,Linhua Hu,Jun Zhu

The role of remnant PbI2 in CH3NH3PbI3 films is still controversial, some investigations have revealed that the remnant PbI2 plays a passivation role, reduces the charge recombination in perovskite solar cells (PSCs), and improves the performance of PSCs, but the opposing views state that remnant PbI2 has no passivation effect and it would deteriorate the stability of the devices. In our investigation, the CH3NH3PbI3 films have been prepared by a two-step spin-coating method and the content of the remnant PbI2 in CH3NH3PbI3 films has been tuned by varying the preparation temperature. It has been found that increasing the heating temperature could increase the coverage of spin-coated PbI2 films, which has led to high coverage CH3NH3PbI3 films and more remnant PbI2 in CH3NH3PbI3 films, and as a result, the performance of PSCs was enhanced obviously and the maximum power conversion efficiency of 14.32 ± 0.28% was achieved by the PSCs prepared at 130/120 °C (PbI2 films were heated at 130 °C and CH3NH3PbI3 films were heated at 120 °C). Furthermore, the dark current, electrochemical impedance spectroscopy and time-resolved fluorescence emission decay measurements revealed that the charge recombination in PSCs has been gradually suppressed and the fluorescence emission lifetime has gradually increased with the content of remnant PbI2 increasing. Thus, the passivation effects of the unreacted and decomposed PbI2 in improving the performance of PSCs have been confirmed unquestionably.

研究领域: 材料科学 · 光伏技术 · 太阳能
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Journal of Physical Chemistry Letters · 2021 · IF 6.475

A Green Lead Recycling Strategy from Used Lead Acid Batteries for Efficient Inverted Perovskite Solar Cells

Lisha Xie,Qiang Zeng,Qingya Li,Shurong Wang,Linhong Li,Zhenyu Li,Fangyang Liu,Xiaojing Hao,Feng Hao

Lead is widely used as a crucial elemental for lead acid batteries (LABs) and emerging halide perovskite solar cells (PSCs). However, the use of soluble lead will raise environmental concerns. For the purpose of Pb recycling, herein, we report a reactant-recycling strategy to extract Pb from used LABs and synthesize high-purity PbI2. The recycled PbI2 shows smaller grain size, higher crystallinity, and higher thermal stability compared to the commercial sources. Perovskite films deposited with the high-quality PbI2 show larger grain size and fewer defects than the commercial ones. Consequently, the synthesized PbI2 enables a power conversation efficiency of 20.45% for the inverted MAPbI3 (MA= methylammonium) PSCs with excellent air stability. This work offers a novel strategy for lead recovery from LABs and a green path for the realization of high-performance PSCs with high defect tolerance.

研究领域: 材料科学 · 环境科学 · 能源技术 · 纳米技术
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ACS Applied Nano Materials · 2022 · IF 6.14

Decorating MoS2 Nanoscrolls with Solution-Processed PbI2 Nanocrystals for Improved Photosensitivity

Zhikang Wu,Feifei Li,Huihui Ye,Xiao Huang,Hai Li

Despite their excellent properties, the low light absorption efficiency of atomically thin transition metal dichalcogenide (TMDC) nanosheets limits their application in optoelectronics. Many efforts have been devoted to enhance the light–matter interaction of the TMDC nanosheets. Among them, coupling the TMDC nanosheet with photoactive materials has drawn extensive attention. Recently, forming one-dimensional nanoscrolls from monolayer TMDC nanosheets has also been proven to be an effective way of improving the photodetection performance of TMDC nanosheets. Herein, photoactive PbI2 nanocrystals were first deposited on a monolayer MoS2 nanosheet grown by chemical vapor deposition using a solution processing method (referred to as PbI2/MoS2). After PbI2/MoS2 was immersed into a mixture of ammonia and isopropanol, PbI2/MoS2 nanoscrolls with sizes of up to several tens of micrometers were formed in a short time. The density of PbI2 nanocrystals on the MoS2 nanosheet was highly dependent on the concentration and immersion time in PbI2 solution. Atomic force microscopy, optical microscopy, high-resolution transmission electron microscopy, X-ray photoelectron spectroscopy, and Raman spectroscopy were used to characterize the PbI2/MoS2 nanosheet and nanoscroll. The as-prepared PbI2/MoS2 nanosheet and nanoscroll showed photosensitivities 2 orders of magnitude higher than those of the MoS2 nanosheet and nanoscroll in visible light, which could be attributed to the type II heterointerface in the PbI2/MoS2 nanosheet and multiple PbI2/MoS2 heterointerfaces in the scrolled structure. Our work indicates that the PbI2 nanocrystal-decorated MoS2 nanoscroll could be a promising candidate for high-performance optoelectronic devices.

研究领域: 纳米材料 · 光电子学 · 纳米光子学 · 材料科学
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