Stable Perovskite Solar Cells Research Articles

MgAc2-Modified SnO2 Electron Transport Layer for Highly Efficient and Thermal Stable Perovskite Solar Cells.

There are always defects and oxygen vacancies in SnO2 prepared by solution methods, hindering efficient carrier transfer between SnO2 and the perovskite in perovskite solar cells. Thus, we employed MgAc2 to modify the interface. Carboxyl groups of MgAc2 filled the oxygen vacancies in SnO2, reducing its surface defect density, and Mg2+ partially replaced surface Sn4+, improving the properties of the SnO2 layer. Finally, perovskite solar cells modified with MgAc2 exhibited a significant improvement in open-circuit voltage and fill factor, improving the power conversion efficiency from 20.52% to 22.02%. Moreover, MgAc2-devices maintained 80% of the initial efficiency after 1250 h in thermal stability tests at 85 °C and 30% relative humidity compared to control devices. This work provides a method for treating the SnO2 electron transport layer and demonstrates the synergistic effects of Mg2+ and acetate ions, which can facilitate the development of efficient and stable perovskite solar cells.

Ligand Assisted Hydrogen Bonding: A Game-Changer in Lead Passivation and Stability in Perovskite Solar Cells.

Lead halide perovskite solar cells (PSCs) have demonstrated power conversion efficiencies comparable to silicon-based solar cells, yet their instability under environmental stressors, such as humidity, heat, and light, remains a significant barrier to commercialization. A primary cause of this instability is the uncoordinated lead ions (Pb2+), which accelerates the degradation of PSCs and pose environmental concerns due to potential lead leakage. Recently, the introduction of ligands into PSCs has shown promise in mitigating lead toxicity through effective passivation, primarily by forming hydrogen bonds (H-bonds) between functional groups of the ligands and the perovskite structure. In this minireview, we explore the critical role of H-bonds in stabilizing PSCs by enhancing the structural integrity of the perovskite layer and reducing lead leakage. Furthermore, we discuss the contribution of these ligands in defect passivation, hydrophobicity, self-encapsulation, cross-linking, and self-healing mechanisms. These insights will highlight the multi-functional capabilities of ligands in improving the long-term stability and durability of PSCs, offering pathways to address current challenges in their commercialization.

Ligand Assisted Hydrogen Bonding: A Game‐Changer in Lead Passivation and Stability in Perovskite Solar Cells

Lead halide perovskite solar cells (PSCs) have demonstrated power conversion efficiencies comparable to silicon‐based solar cells, yet their instability under environmental stressors, such as humidity, heat, and light, remains a significant barrier to commercialization. A primary cause of this instability is the uncoordinated lead ions (Pb2+), which accelerates the degradation of PSCs and pose environmental concerns due to potential lead leakage. Recently, the introduction of ligands into PSCs has shown promise in mitigating lead toxicity through effective passivation, primarily by forming hydrogen bonds (H‐bonds) between functional groups of the ligands and the perovskite structure. In this minireview, we explore the critical role of H‐bonds in stabilizing PSCs by enhancing the structural integrity of the perovskite layer and reducing lead leakage. Furthermore, we discuss the contribution of these ligands in defect passivation, hydrophobicity, self‐encapsulation, cross‐linking, and self‐healing mechanisms. These insights will highlight the multi‐functional capabilities of ligands in improving the long‐term stability and durability of PSCs, offering pathways to address current challenges in their commercialization.

Low-cost green antisolvent with an ultrawide processing window for efficient and stable perovskite solar cells

Antisolvent engineering is one of the most useful strategies to get high-efficiency perovskite solar cells (PSCs). Nevertheless, the most present commonly used effective antisolvents, such as chlorobenzene and diethyl ether, are toxic and expensive. Moreover, these antisolvents applied in PSCs are rather restricted due to their narrow processing window. Herein, we report a low-cost green antisolvent isopropanol (IPA) that displays ultrawide processing window, which dramatically enhances the reproducibility of PSCs. The highest power conversation efficiency of PSCs treated by IPA can reach as high as 24.8%. The origin of IPA effects is further disclosed by the intermolecular hydrogen-bonding force between IPA and DMF/DMSO, and the force can effectively remove DMF/DMSO in the spinning perovskite precursor film and helpfully enhance perovskite crystal growth with less carrier recombination as demonstrated by using various techniques. Our results here demonstrate a cheap green antisolvent for reproducible, high-efficient, stable PSCs and also provide an in-depth understanding the significant role of antisolvent in the fabrication of PSCs.

A Pyrrole Modified 3,4-Propylenedioxythiophene Conjugated Polymer as Hole Transport Layer for Efficient and Stable Perovskite Solar Cells.

Despite the outstanding electric properties and cost-effectiveness of poly(3,4-ethylenedioxythiophene) (PEDOT) and its derivatives, their performance as hole transport layer (HTL) materials in conventional perovskite solar cells (PSCs) has lagged behind that of widely used spirobifluorene-based molecules or poly(triaryl amine). This gap is mainly from their poor solubility and energy alignment mismatch. In this work, the design and synthesis of a pyrrole-modified HTL (PPr) based on 3,4-propylenedioxythiophene (ProDOT) are presented for efficient and stable PSCs. As a result of the superior defects passivation ability, excellent contact with perovskite, enhanced hole extraction, and high hydrophobicity, the unencapsulated PPr-based PSCs showed the peak PCE of 21.49% and outstanding moisture stability (over 4000 h). This work highlights the potential application of ProDOT-based materials as HTL for PSCs and underscores the importance of the rational design of PEDOT and its derivatives.

Synergistic Passivation of Bulk and Interfacial Defects Improves Efficiency and Stability of Inverted Perovskite Solar Cells

Defects both in bulk and at the interfaces serve as charge trapping sites for nonradiative recombination and as ion migration pathways, resulting in degradation of perovskite solar cell efficiency and stability. In this work, a strategy for simultaneous passivation of both bulk and interfacial defects is reported. For bulk passivation polystyrene (PS) is used as an additive in the perovskite precursor which reduces the structural defects by forming larger defect‐free grains. While the F‐PEAI cation is used to passivate the interfacial defects, present at both perovskite HTL/ETL interfaces. Furthermore, by conducting control measurements with just bulk modification (PS), just interface modification (F‐PEAI), and a combination of both, the role of individual defect passivation strategies is decoupled. As a result of simultaneous bulk as well as interfacial passivation, the modified perovskite solar cell shows the highest efficiency of 22.32% with a high Voc of 1.14 V and fill factor of 80%. Moreover, the cells have excellent stability retaining 92% and 99% of their initial efficiency after 1008 h and 560 h under ISOS‐ D1 and D2 storage conditions. These results highlight the importance of simultaneous bulk and interfacial passivation for improving solar cell efficiency and stability.

Molybdenum-Oxide-Modified PEDOT:PSS as Efficient Hole Transport Layer in Perovskite Solar Cells

Over the last ten years, there has been a remarkable enhancement in the power conversion efficiency (PCE) of perovskite solar cells (PSCs), with poly (3,4-ethylenedioxythiohene):poly (styrenesulfonate) (PEDOT:PSS) emerging as a prevalent choice for the hole transport layer (HTL). Nevertheless, the evolution of the widely utilized PEDOT:PSS HTL has not kept pace with the swift advancements in PSC technology, attributed to its suboptimal electrical conductivity, acidic nature, and inadequate electron-blocking performance. This study presents a novel approach to enhance the HTL by introducing molybdenum oxide (MoO3) into the PEDOT:PSS, leveraging the conductivity and solution processing compatibility of MoO3. Two methods for MoO3 integration were explored: an ammonium molybdate tetrahydrate (AMT) precursor and the direct addition of MoO3 nanoparticles. The carrier dynamics of PSCs modified by MoO3 are significantly optimized. Therefore, the PCE of the device modified by AMT and molybdenum oxide is increased to 18.23 and 19.64%, respectively, and the stability of the device is also improved. This study emphasizes the potential of MoO3 in contributing to the development of more efficient and stable PSCs.

How the Spacer Influences the Stability of 2D Perovskites?

Two-dimensionallead halide perovskites (2D HPs) represent as an emerging class of materials given their tunable optoelectronic properties and long-term stability in perovskite solar cells. However, the ever-growing field of optoelectronic devices using 2D HPs requires fundamental understanding of the influence of the spacer on the physiochemical properties and stability of perovskites as well as establish which cation properties are closely related to suppress the halogen ion mobility. This study focuses on investigating the influence of organic spacers with intrinsic properties (e.g., rigidity and flexibility, special groups) and variations of material dimensions on the stability of halogen ions and inorganic frameworks in 2D HPs. It is found that the perovskite structure composed of rigidity molecules owns better stability of halogen ion and inorganic framework than that of flexible molecules. The stability of ions exhibits a negative correlation with the dimensions of perovskite. More importantly, a simple descriptor for measuring the stability of halogen ions in 2D HPs is constructed. By causal discovery algorithms with more physical and chemical significance, the Kappa shape index, number of rotatable bonds, and aromatic carbocycles in organic spacers are identified as causal and important features for the stability of halogen ions in 2D HPs.

Air-Processed Efficient Perovskite Solar Cells With Full Lifecycle Management.

Despite the outstanding power conversion efficiency of perovskite solar cells (PSCs) realized over the years, the entire lifecycle from preparation and operation to discarding of PSCs still needs to be carefully considered when it faces the upcoming large-scale production and deployment. In this study, bio-derived chitin-based polymers are employed to realize the full lifecycle regulation of air-processed PSCs by forming multiple coordinated and hydrogen bonds to stabilize the lead iodide and organic salt precursor inks, accelerating the solid-liquid reaction and crystallization of two-step deposition process, then achieving the high crystalline and oriented perovskites with less notorious charge defects in the open air. The air-prepared PSCs exhibit a decent efficiency of 25.18% with high preparation reproducibility and improved operational stability toward the harsh environment and mechanical stress stimuli. The modified PSCs display negligible fatigue behavior with keeping 92% of its initial efficiency after operating for 32 diurnal cycles (ISOS-LC-1 protocol). Meanwhile, closed-loop lead management of end-of-life PSCs including suppression of lead leakage, toxicity evaluation of broken devices, and recycling of lead iodide components are comprehensively investigated. This work sheds light on a promising avenue to realize the entire lifecycle regulation of air-processed efficient and stable PSCs.

Bimolecular Passivation-Dipole Bridge for Highly Efficient Inverted Perovskite Solar Cells with Low Nonradiative Recombination Loss.

Constructing charge-selective heterointerface with minimized defect state and matched energy level alignment is essential to reduce nonradiative recombination for achieving high-performance perovskite solar cells (PSCs). Herein, a bimolecular passivation-dipole bridge comprised of sodium phenylmethanesulfonate (SPM) and 2-phenylethylammonium iodide (PEAI) is carefully developed to regulate perovskite heterointerface. SPM passivates defect states and upshifts Fermi level (EF) of perovskite surface, and subsequent PEAI further induces additional negative dipole and causes the surface EF of perovskite pinning to negative polaron transport state of electron transport layer PCBM, which significantly promotes electron extraction at the perovskite electron-selective contact. These advantages are confirmed by a remarkably improved efficiency from 21.74% for control to 25.12% for treated PSC with excellent stability. Moreover, corresponding nonradiative recombination loss impressively diminishes from 123 to 70 meV, and charge transport-induced fill factor loss is only 3.00%. This work provides a promising approach via passivation-energetic synergy for engineering perovskite heterointerface toward highly efficient and stable PSCs.

Iodide Management and Oriented Crystallization Modulation for High-Performance All-Air Processed Perovskite Solar Cells.

Halide-related defects at the buried interface not only cause nonradiative recombination, but also seriously impair the long-term stability of perovskite solar cells (PSCs). Herein, a bottom-up, all-in-one modification strategy is proposed by introducing a multisite antioxidant ergothioneine (EGT) at the buried interface to manage iodide ions and manipulate crystallization dynamics. The findings demonstrate that EGT not only passivates uncoordinated Sn4+/Pb2+ defects, but also firmly anchors iodide ions and inhibits their oxidation to I2. Additionally, the modification by EGT enhances the oriented crystallization of perovskite, improves the carrier dynamics, and releases residual stresses. Consequently, the optimized all-air processed device (Rb0.02(FA0.95Cs0.05)0.98PbI2.91Br0.03Cl0.06) achieves a remarkable power conversion efficiency (PCE) of 25.13%, which is among the highest values reported for devices fabricated in air, along with ultrahigh open-circuit voltage (VOC) of 1.191V and fill factor (FF) of 84.9%. The optimized device without encapsulation exhibits strong humidity, thermal, and operational stability under ISOS protocol. Specifically, the initial efficiency of the device is retained at 90.12% after 1512 h of thermal ageing at 65°C and 90.14% after 930 h of continuous maximum power point tracking (MPPT) under simulated AM1.5 illumination.

π-Conjugation-Induced In Situ Nanoscale Ordering of Spiro-OMeTAD Boosts the Efficiency and Stability of Perovskite Solar Cells.

Spiro-OMeTAD hole transport materials typically exhibit an amorphous state in perovskite solar cells. However, the lack of structural ordering leads to weak intermolecular interaction, inferior carrier transfer, and poor stability in devices. Herein, we developed a π-conjugation-induced short-range ordering strategy to modulate the stacking order of spiro-OMeTAD during film formation. A clear molecular ordering at the nanoscale is observed, which enhances intermolecular π-π stacking in spiro-OMeTAD and enables effective carrier extraction and favorable energy level alignment. The nanoscale-ordered spiro-OMeTAD allows the achievement of perovskite solar cells with a champion efficiency of 25.37%, surpassing devices utilizing amorphous spiro-OMeTAD (23.52%). The unencapsulated device demonstrates enhanced operational stability by retaining 98% of its initial efficiency under continuous 1 sun equivalent illumination at 60 °C for 840 h. This work establishes a significant and valid modulation concept for the stacking order of organic transport materials, paving the way for the development of efficient and stable perovskite solar cells.

Surface Reaction Induced Compressive Strain for Stable Inorganic Perovskite Solar Cells

AbstractCesium‐based inorganic perovskites have emerged as promising light‐harvesting materials for perovskite solar cells (PSCs) due to their promising thermal‐ and photo‐stability. However, obstacles to commercialization remain regarding their phase instability. In this work, we report a facile and effective strategy to regulate the surface compressive strain via in situ surface reaction to stabilize CsPbI3 perovskite. The use of a chelating ligand with a molecular configuration closely matching the integer multiples of the unit cell lattice parameters of CsPbI3 induces compressive strain at the surface of CsPbI3. The chemical bonding and strain modulation synergistically not only passivate film defects, but also inhibit perovskite phase degradation, thus significantly improving the intrinsic stability of inorganic perovskite. Consequently, enhanced power conversion efficiency (PCE) of 21.0 % and 18.6 % were respectively achieved in 0.16‐cm2 lab‐scale devices and 25.3‐cm2 solar modules. Further, surface reaction enables PSCs with enhanced thermal and operational stability; these devices retain over 95 % of their initial PCE after damp‐heat tests (i.e., in 85 °C and 85 % R. H. air) for 2000 h, and remain 99 % of their initial PCE after operating for 2000 h, representing one of the most stable inorganic PSCs reported so far.

Synthesis of Multifunctional Organic Molecules via Michael Addition Reaction to Manage Perovskite Crystallization and Defect

AbstractAdditive engineering plays a pivotal role in achieving high‐quality light‐absorbing layers for high‐performance and stable perovskite solar cells (PSCs). Various functional groups within the additives exert distinct regulatory effects on the perovskite layer. However, few additive molecules can synergistically fulfill the dual functions of regulating crystallization and passivating defects. Here, we custom‐synthesized 2‐ureido‐4‐pyrimidone (UPy) organic small molecules with diverse functional groups as additives to modulate crystallization and defects in perovskite films via the Michael addition reaction. Theoretical and experimental investigations demonstrate that the −OH groups in UPy exhibit significant effects in fixing uncoordinated Pb2+ ions, passivation of lead‐iodide antisite defects, alleviating hysteresis, and reducing non‐radiative recombination. Furthermore, the enhanced C=O and −NH2 motifs interact with the A‐site cation via hydrogen bonding, which relieves residual strain and adjusts crystal orientation. This strategy effectively controls perovskite crystallization and passivates defects, ultimately enhancing the quality of perovskite films. Consequently, the open‐circuit voltage of the UPy‐based p‐i‐n PSCs reaches 1.20 V, and the fill factor surpasses 84 %. The champion device delivers a power conversion efficiency of 25.75 %. Remarkably, the unencapsulated device maintained 96.9 % and 94.5 % of its initial efficiency following 3,360 hours of dark storage and 1,866 hours of 1‐sun illumination, respectively.

Improved Charge‐Transfer Doping in Crystalline Polymer for Efficient and Stable Perovskite Solar Cells

AbstractPerovskite solar cells (PSCs) have significant potential for next‐generation photovoltaic technology applications. However, the instability of hole transport layers (HTLs) becomes the major obstacle to long‐term operational devices, which are affected by the intrinsic thermal instability and loose structure of hole transport materials, as well as the hygroscopicity and migration of dopants. Here, poly(3‐hexylthiophene‐2,5‐diyl) (P3HT) is used as a model crystalline polymer to thoroughly investigate effective p‐type doping strategies and the underlying mechanism. According to Hard–Soft‐Acid–Base theory, the soft base P3HT is more likely to form a stable Lewis acid–base adduct with the reactive soft acid radical, resulting in a strong charge‐transfer interaction, thereby enhancing conductivity and regulating the energy band of the HTL. Meanwhile, the radical cation salt can promote pre‐nucleation to optimize the crystallization orientation of P3HT. The resulting PSCs exhibited the efficiency of 25.16%, which is the highest efficiency reported so far based on doped P3HT. In addition, the resulting devices demonstrated excellent stability, maintaining 96.5%, 96%, and 91% of their initial efficiency after aging under continuous illumination for 2028 h, at 85 °C for 1080 h, and at maximum power point (MPP) tracking under continuous 1 Sun illumination at 85 °C for 528 h, respectively.

Enhanced optoelectronic characteristics of La-doped ZnO and its compatibility with Cs-doped MAPbI3 perovskite absorber material

Abstract The present study investigates the structural, electrical and optical characteristics of pristine and lanthanum (La)-doped zinc oxide electron transport layers (ETLs) fabricated by the sol gel method and their compatibility with Cs0.10MA0.90Pb(I0.9Br0.10)3 absorber layer for perovskite solar cells. All the ETLs were deposited under same deposition conditions, with the only difference in La percentage in the precursor solutions, ranging from 0 to 6%. X-ray diffraction (XRD) analysis demonstrated the presence of crystalline ZnO thin films and the absence of any impurity phases after La-doping. The calculated crystallite size, determined using Scherrer’s equation, increased from 11.13 to 21.76 nm after the introduction of dopant. The doping with 4% La led to the decrease in the optical bandgap from 3.32 eV of pristine ZnO to 3.23 eV. SEM analysis revealed better morphology of perovskite/4% La:ZnO specimen, which facilitated the absorbance and reduced the charge carrier recombination. It also exhibited superior resilience towards moisture and humidity which will eventually contribute to the development of more stable and efficient planar perovskite solar cells (PCSs).

Microscopic analysis of low but stable perovskite solar cell device performance using electron spin resonance

Perovskite solar cells have attracted much attention as next-generation solar cells. However, a typical hole-transport material, spiro-OMeTAD, has associated difficulties including tedious synthesis and high cost. To overcome these shortcomings, an easily synthesized and low-cost hole-transport material has been developed: HND-2NOMe. Although HND-2NOMe has high local charge mobility because of the quasi-planar structure, its lower device performance is a weak point, the cause of which has not yet been clarified. Here, we analyse the source of the lower performance by clarifying the internal states from a microscopic viewpoint using electron spin resonance. We observe hole diffusion from perovskite to HND-2NOMe under dark conditions, indicating hole barrier formation at the perovskite/HND-2NOMe interface, leading to lower performance. Although such a barrier is formed, less hole accumulation for the HND-2NOMe-based cells under solar irradiation occurs, which is related to the stable performance. The sources of the lower but stable performance are crucially important for providing guidelines for improving the device performance.

Efficient and stable inverted perovskite solar cells enabled by homogenized PCBM with enhanced electron transport

Fullerene derivatives are extensively employed in inverted perovskite solar cells due to their excellent electron extraction capabilities. However, [6,6]-phenyl-C61-butyric acid methyl ester (PCBM) agglomerates easily in solution and exhibits a relatively low ionization barrier, increasing charge recombination losses and charge accumulation in the interface. Here, tetramethylthiuram disulfide (TMDS) is introduced into the PCBM solution to induce the formation of reducing sulfur radicals through UV light irradiation, allowing for n doping of the PCBM material. The resulting modified PCBM layer exhibits enhanced conductivity and electron mobility, significantly suppressing charge recombination. As a result, the resulting devices incorporating TMDS achieve a champion efficiency of 26.10% (certified 25.39%) and 24.06% at a larger area (1.0 cm2) with negligible hysteresis. More importantly, the optimized devices retain 95% and 90% of their initial efficiency after 1090 h under damp heat testing (85 °C and 85% relative humidity) and after 1271 h under maximum power point-tracking conditions, respectively.

Accelerating Additive-Assisted Defect Passivation via the Structural Isomer Effect for Highly Efficient and Stable Perovskite Solar Cells.

Defects in hybrid perovskites have hindered the development of highly efficient and stable hybrid perovskite solar cells (PSCs). Therefore, researchers have used additives to passivate defects in hybrid perovskites; however, detailed studies on multifunctional group additives with structural isomers are limited. In this letter, we report the improved defect passivation ability of additives through the structural isomer effect and enhanced photovoltaic performance using this effect. l-Alanine methyl ester hydrochloride (l-AMECl) and its structural isomer, β-AMECl, were used to understand the influence of structural variations in functional groups. The structural isomer β-AMECl effectively reduced the trap density in the hybrid perovskite, thereby enhancing the photovoltaic parameters. Consequently, we achieved a power conversion efficiency of 24.25% with β-AMECl, which is the best result among PSCs using additives. Additionally, the PSCs with β-AMECl maintained an initial efficiency of 94% over 2500 h at 25 °C and 25% relative humidity, showing improved long-term stability.

Modifying the buried interface by a sulfamate enable efficient perovskite solar cells with high stability

The buried interface between the pivotal perovskite layer and the electron transfer layer (ETL) greatly affects the photoelectric property of perovskite layer and the final performance of a perovskite solar cell (PSC). Effectively modifying the buried interface is feasible to improve the photoelectric conversion efficiency (PCE) and stability of PSCs. Herein, we employ a sulfamate sodium 4-aminoazobenzene-4′-sulfonate (SABS) with zwitterion to modify the SnO2 film surface to improve the performance of PSCs. The post-treatment makes the surface of SnO2 film smoother and also passivate the anion and cation vacancies of SnO2, which are benefit to the growth of perovskite crystals and strengthen the interface contact between SnO2 layer and perovskite layer. Furthermore, SABS molecules can passivate defects of perovskite layer at the buried interface. By using this post-treating method, the PCE of the final PSC is increased from 21.76 % to 23.86 %, and the storage and operational stability are also significantly improved. This promotion the buried interface via post-treating the SnO2 film with a zwitterion passivator provides a convenient strategy to effectively improve the performance and stability of PSCs.