Champion Power Conversion Efficiency Research Articles

Photothermal Welding Strategy for Mechanical Stability and High Efficiency of ETL‐Free f‐PSCs

AbstractFlexible perovskite solar cells (f‐PSCs) have drawn widespread interest owing to their distinguished advantages in excellent flexibility and relatively low cost. However, the brittle grain boundaries (GBs) and defects in flexible perovskite film tremendously influence the power conversion efficiency (PCE) and mechanical flexibility of f‐PSCs. Herein, photothermal welding, a novel method, is used to improve the perovskite films quality and the PCE of f‐PSCs with a near‐infrared (NIR) dye (indocyanine green, ICG) and polycaprolactone (PCL) as additives. Due to the strong photothermal effect, ICG molecule not only can significantly enhance NIR light harvesting, but it also can weld GBs upon exposure to an NIR laser, which is conducive to the GBs connections and device flexibility. Meanwhile, the S═O bond of ICG and C═O bond of PCL can simultaneously coordinate with Pb2+ defects in perovskite. Furthermore, they can control crystal growth to form a smooth surface of perovskite film. Consequently, the unencapsulated PSCs based on ICG/PCL displays a high champion PCE of 20.62%, with 88.4% of the original PCE after being placed in dark conditions for 600 h. The f‐PSCs delivers a champion PCE of 19.55% and exhibits excellent mechanical stability, thus providing a meaningful scientific direction to fabricate high‐flexible f‐PSCs.

In-Situ Self-Assembly Dipole Shielding Layer Toward Efficient and Stable Inorganic Perovskite Solar Cells.

Despite CsPbI2.75Br0.25inorganic perovskites exhibit high potential for single-junction and/or tandem solar cells, unexpected non-radiative recombination, and mismatched interfacial band alignment within the inorganic perovskite solar cells (PSCs) disadvantageously affect their photovoltaic performance. Rational design of the dipole shielding layer (DSL) is vital to realize a win-win situation for the defect passivation and band alignment. Herein, A-site dipole molecules, that is, neopentylamine and 2-methylbutylamine, are employed for in-situ self-assembly of a thus-far unreported DSL at the interface between 3D perovskite and hole transport layer. The as-prepared DSL demonstrates a 2D RP phase perovskite and the lattice-matching structurally-stable DSL@3D perovskite enables to alleviate the unexpected surface defects and suppress the spontaneous non-radiative recombination by means of effectively tuning the surface work function via regulating the dipole moment length and Van der Waals gap. Accordingly, the top dipole-modified inorganic PSCs exhibit a champion power conversion efficiency (PSC) as high as 19.77% and a fill factor over 83%. Equally importantly, the corresponding solar cells demonstrate a remarkable enhanced stability, maintaining 90% of its initial efficiency for more than 1200h without encapsulation under a 20% ± 5% relative humidity.

Perovskite solar cells with self-disintegrating seeds deliver an 83.64 % fill factor

Large-seed-induced regulation significantly impacts perovskite film grain growth; however, it inadequately addresses stress and defect issues at the perovskite interface. To counter this, we introduce an innovative self-disintegrating seed approach, employing 2D (4-FBZA)2PbI4 perovskite to enhance the crystallization process. During perovskite crystal growth, (4-FBZA)2PbI4 could disintegrate and release 4-FBZA+ ions. These ions effectively anchor the perovskite interface and interact with FA+ and [PbI6]4- within the lattice, passivating defects and releasing detrimental stress. This strategy results in reduced nonradiative recombination and residual stress, culminating in perovskite solar cells (PSCs) achieving a champion power conversion efficiency (PCE) of 23.73 % and a remarkable fill factor of 83.64 %. Crucially, unencapsulated PSCs retain over 90 % of their initial PCE following 2000 h of exposure in ambient conditions at 25±5 °C and 60 % relative humidity.

Interfacial engineering with a ferrocene derivative for air-stable inverted perovskite solar cells with high fill factor of 83.57 %

Perovskite solar cells have demonstrated exceptional photovoltaic performance, but stability remains a challenge due to insufficient interfaces. In this work, a UV-resistance ferrocene derivative, 1,1′-bis (diphenylphosphine) ferrocene (DPPF), is introduced between the electron transport layer and the perovskite, reducing defect density by interaction with undercoordinated Pb2+, suppressing non-radiative recombination of charge carriers, and enhancing electron extraction. Desirable interfacial properties and homogeneous perovskite grains are formed, resulting in a champion power conversion efficiency (PCE) of 20.82 % and a significantly improved fill factor of 83.57 %. Moreover, DPPF can optimize the interfaces, provide a brand-new morphology with exceptional air durability, cover the active layer to restrain water and oxygen intrusion, and suppress metal electrode corrosion. Resultant devices without encapsulation have remained above 80 % of their initial PCE for 1400 h under 25 °C air and 50–60 % relative humidity conditions.

Designed Additive to Regulated Crystallization for High Performance Perovskite Solar Cell

It is a crucial role for enhancing the power conversion efficiency (PCE) of perovskite solar cells (PSCs) to prepare high‐quality perovskite films, which can be achieved by delaying the crystallization of perovskite film. Hence, we designed difluoroacetic anhydride (DFA) as an additive to regulating crystallization process thus reducing defect formation during perovskite film formation. It was found DFA reacts with DMSO by forming two molecules, difluoroacetate thioether ester (DTE) and difluoroacetic acid (DA). The strong bonding DTE·PbI2 and DA·PbI2 retard perovskite crystallization process for high‐quality film formation, which was monitored through in situ UV‐vis and PL tests. By using DFA additives, we prepared perovskite films with high‐quality and low defects. Finally, a champion PCE of 25.28% was achieved with excellent environmental stability, which retained 95.75% of the initial PCE after 1152 h at 25 °C under 25% RH.

Side‐chain symmetry‐breaking strategy on porphyrin donors enables high‐efficiency binary all‐small‐molecule organic solar cells

AbstractSide‐chain symmetry‐breaking strategy plays an important role in developing photovoltaic materials for high‐efficiency all‐small‐molecule organic solar cells (ASM OSCs). However, the power conversion efficiencies (PCEs) of ASM OSCs still lag behind their polymer‐based counterparts, which can be attributed to the difficulties in achieving favorable morphology. Herein, two asymmetric porphyrin‐based donors named DAPor‐DPP and DDPor‐DPP were synthesized, presenting stronger intermolecular interaction and closer molecular stacking compared to the symmetric ZnP‐TEH. The DAPor‐DPP:6TIC blend afforded a favorable morphology with nanoscale phase separation and more ordered molecular packing, thus achieving more efficient charge transportation and suppressed charge recombination. Consequently, the DAPor‐DPP:6TIC‐based device exhibited superior photovoltaic parameters, yielding a champion PCE of 16.62% higher than that of the DDPor‐DPP‐based device (14.96%). To our knowledge, 16.62% can be ranked as one of the highest PCE values among the binary ASM OSC filed. This work provides a prospective approach to address the challenge of ASM OSCs in improving film morphology and further achieving high efficiency via side‐chain symmetry‐breaking strategy, exhibiting great potential in constructing efficient ASM OSCs.

Designed Additive to Regulated Crystallization for High Performance Perovskite Solar Cell.

It is a crucial role for enhancing the power conversion efficiency (PCE) of perovskite solar cells (PSCs) to prepare high-quality perovskite films, which can be achieved by delaying the crystallization of perovskite film. Hence, we designed difluoroacetic anhydride (DFA) as an additive to regulating crystallization process thus reducing defect formation during perovskite film formation. It was found DFA reacts with DMSO by forming two molecules, difluoroacetate thioether ester (DTE) and difluoroacetic acid (DA). The strong bonding DTE·PbI2 and DA·PbI2 retard perovskite crystallization process for high-quality film formation, which was monitored through in situ UV-vis and PL tests. By using DFA additives, we prepared perovskite films with high-quality and low defects. Finally, a champion PCE of 25.28% was achieved with excellent environmental stability, which retained 95.75% of the initial PCE after 1152 h at 25 °C under 25% RH.

3D Conjugated Hole Transporting Materials for Efficient and Stable Perovskite Solar Cells and Modules.

The orthogonal structure of the widely used hole transporting material (HTM) Spiro-OMeTAD imparts isotropic conductivity and excellent film-forming capability. However, inherently weak intra- and inter-molecular π-π interactions result in low intrinsic hole mobility. Herein, a novel arylamine derivative, termed FTPE-ST, with a twist conjugated dibenzo[g,p]chrysene core and coplanar 3,4-ethylenedioxythiophene (EDOT) as extended donor units, was designed to enhance intra- and inter-molecular π-π interactions, without compromising on solubility. The 3D configuration provides the material multi-direction charge transport as well as excellent solubility even in 2-methylanisole (2-MA), and its large conjugated delocalization backbone endows the HTM with a high hole mobility (7.2 × 10-4 cm2V-1s-1). Moreover, the sulfur donors in the EDOT units coordinate to lead ions on the perovskite surface, leading to stronger interfacial interactions and the suppression of defects at the perovskite/HTM interface. As a result, perovskite solar cells (PSCs) employing FTPE-ST as the HTM achieve a champion power conversion efficiency (PCE) of 25.21% with excellent long-time stability, which is one of the highest PCEs for non-spiro HTMs in n-i-p PSCs. In addition, the excellent film-forming capacity of the HTM enables the fabrication of FTPE-ST-based large-scale PSCs (1.0 cm2) and modules (29.0 cm2), which achieve PCEs of 24.21% (certificated 24.17%) and 21.27%, respectively. This article is protected by copyright. All rights reserved.

Side Chain Functional Molecule Additives for Efficient and Stable Perovskite Solar Cells

AbstractIn the commercial development of perovskite solar cells, the main challenge lies in achieving efficient devices with high stability. Additive engineering in polycrystalline perovskites is considered as an effective approach to address this challenge by passivating surface defects and reducing carrier losses associated with these defects. In this work, the passivation effect of molecules with different side chain groups on perovskites and the role of binding energy in mitigating carrier loss are studied. The findings reveal that the thiophene group is particularly effective in passivating defects and enhancing hole transport. Consequently, devices treated with 2‐thienylmethylamine hydrochloride (TMAC) demonstrate a champion power conversion efficiency (PCE) of 24.63%. Furthermore, these TMAC‐treated devices exhibit remarkable stability, maintaining over 93.13% of their initial efficiencies after 1200 h of continuous illumination under maximum power point tracking (MPPT). This research presents a pathway to enhance the optoelectronic performance and stability of perovskite solar cells.

Bifunctional passivation by lewis-base molecules for efficient printable mesoscopic perovskite solar cells

Printable mesoscopic perovskite solar cells (PM-PSCs) possess notable merits in terms of cost-effectiveness, easy manufacturing, and large scale applications. Nevertheless, the absence of a hole transport layer contributes to the exacerbation of carrier recombination, and the defects between the perovskite and electron transport layer (ETL) interfaces significantly decrease the efficiency of the devices. In this study, a bifunctional surface passivation approach is proposed by applying a thioacetamide (TAA) surfactant on the mesoporous TiO2 interface. The results demonstrate that TAA molecules could interact with TiO2, thereby diminishing the oxygen vacancy defects. Additionally, the amino group and sulfur atoms in TAA molecules act as Lewis base to effectively passivate the uncoordinated Pb2+ in perovskite and improve the morphology of perovskite, and decrease the trap-state density of perovskite. The TAA passivation mechanism improves the alignment of energy levels between TiO2 and perovskite, facilitating electron transport and reducing carrier recombination. Consequently, the TAA-passivated device achieved a champion power conversion efficiency (PCE) of 17.86% with a high fill factor (FF) of 79.16% and an open-circuit voltage (VOC) of 0.971 V. This investigation presents a feasible strategy for interfacial passivation of the ETL to further improve the efficiency of PM-PSCs.

Stable and efficient perovskite solar cells based on tert-butyl peroxy-2-ethylhexanoate modified hole transport layer

Nowadays, perovskite solar cells (PSCs) have gained significant attention as one of the most promising new energy technologies. However, the application of spiro-OMeTAD, a highly efficient organic hole transport material (HTM) in PSCs, is limited due to its inherent weaknesses in conductivity and hole mobility. Here, a free radical initiator, tert-butyl peroxy-2-ethylhexanoate (TBPEH) is introduced to induce the rapid and controllable oxidation of Spiro. TBPEH-modified hole transport layer (HTL) produces more free radical cations, increasing carrier mobility and electrical conductivity. A smoother surface of the modified HTL improves the charge transport efficiency. Additionally, trap-state density and defect-induced nonradiative recombination of TBPEH-modified device are decreased. In addition, better energy level matching between the HTL and perovskite layer enables more efficient hole transport. Consequently, the PSC doped with TBPEH achieves a champion power conversion efficiency (PCE) of 24.33%, surpassing the PCE of 21.72% obtained from the pristine device. Furthermore, the TBPEH-modified devices show better stability. Storing in the atmosphere at 30% relative humidity for 42 days, the TBPEH-modified device maintains 90.8% of its highest efficiency, compared to the 73.8% of the pristine one.

Narrow bandgap Sn-Pb perovskite solar cells with high operational stability modulated by imidazoline derivative

Sn-Pb mixed perovskites with narrow bandgap (NBG) are important for high-performance single- and multi-junction perovskite solar cells (PSCs). However, the inherent Sn2+ oxidation and ion migration lead to inferior stability. Herein, 2-hydrazino-2-imidazoline hydrobromide (2H2I) is employed as a coordinating additive to regulate the film crystallization and inhibit Sn2+ oxidation. Meanwhile, 2H2I can form hydrogen bonds with I− ions to suppress ion migration, thereby improving photovoltaic stability. The target FA0.8Cs0.2Sn0.5Pb0.5I3:2H2I PSC exhibits a champion power conversion efficiency (PCE) of 22.44 %, higher than that of the control device (19.16 %). The target devices retain 90 % (T90) and 80 % (T80) of the initial PCE under maximum power point (MPP) tracking for 1360 h at room temperature and for 436 h at 65 °C, respectively, the highest values for NBG Sn-Pb PSCs. This work demonstrates an effective strategy toward photothermally stable Sn-Pb PSCs.

Elimination of Intragrain Defect to Enhance the Performance of FAPbI3 Perovskite Solar Cells by Ionic Liquid.

Ionic liquids have been widely used to improve the efficiency and stability of perovskite solar cells (PSCs), and are generally believed to passivate defects on the grain boundaries of perovskites. However, few studies have focused on the relevant effects of ionic liquids on intragrain defects in perovskites which have been shown to be critical for the performance of PSCs. In this work, the effect of ionic liquid 1-hexyl-3-methylimidazolium iodide (HMII) on intragrain defects of formamidinium lead iodide (FAPbI3) perovskite is investigated. Abundant {111}c intragrain planar defects in pure FAPbI3 grains are found to be significantly reduced by the addition of the ionic liquid HMII, shown by using ultra-low-dose selected area electron diffraction. As a result, longer charge carrier lifetimes, higher photoluminescence quantum yield, better charge carrier transport properties, lower Urbach energy, and current-voltage hysteresis are achieved, and the champion power conversion efficiency of 24.09% is demonstrated. These observations suggest that ionic liquids significantly improve device performance resulting from the elimination of {111}c intragrain planar defects.

A novel chain-like conjugated donor-π-acceptor molecular additive for highly efficient and stable perovskite solar cells

In donor-π-acceptor (D-π-A) molecules, the coordination ability of the acceptor can be enhanced by the directed movement of delocalized electrons (DEs) on the π-bridge. However, the conventional aromatic ring as π-bridge limits the number of DEs due to the structural characteristic, which restrict the coordination ability of the acceptor, and there is still a lack of research on this issue. Herein, we proposed a chain-like conjugated π-bridge design strategy to address this issue. The Astaxanthin with eleven contiguous C − C = C fragments was selected as a chain-like D-π-A additive for perovskite films. Twenty-two DEs in such chain-like bridge can move towards the C = O group by the D-π-A effect within Astaxanthin, which increases the electron cloud density of C = O group so that enhances its coordination capacity with cations. Ultimately, the Astaxanthin-based device achieved a champion power conversion efficiency (PCE) of 24.43 % and maintained more than 95 % and 91 % of initial PCE for aging 1000 h in dry air (RH < 1 %) and atmosphere (RH = 20 ∼ 30 %), respectively. This work provides a novel strategy to break the restriction of aromatic rings to DEs, which provides theoretical and experimental guidance for further designing chain-like D-π-A additives with strong defect passivation ability to boost photovoltaic performance of PSCs.

Delaying crystallization and anchoring the grain boundaries defects via π-π stacked molecules for efficient and stable wide-bandgap perovskite solar cells

Owing to the easy migration of halogen ions in wide-bandgap perovskite, it will lead to the formation of a large number of uncoordinated Pb2+ to form deep-level defects, which seriously affects the power conversion efficiency (PCE) and stability of wide-bandgap perovskite solar cells (PSCs). The introduction of additives has been recognized as an effective method to improve these defects, especially Lewis acid-base additives. Herein, Lewis base molecule dibenzofuran (DBF) with π-conjugated system, which can form π-π stacked dimer, is used as a perovskite additive. The detailed crystallization process of perovskite main precursor triggered by DBF is measured by using laser scanning confocal microscopy. It is demonstrated that the addition of DBF in perovskite samples resulted in a deceleration of the crystallization process, which is due to the formation of Lewis acid-base complexes between DBF π-π stacked dimer and perovskite, which can obtain perovskite films with reduced defect density. As a result, the champion PCE of the wide-bandgap (1.68 eV) perovskite device reaches 20.18 %, significantly higher than the control device (17.79 %). Additionally, the device with no encapsulation demonstrates better stability, as it maintains over 90 % of the initial PCE under an air environment with 30–40 % relative humidity (RH) and 25 °C for 1200 h.

Acceptor molecules with different central and terminal units for P3HT based solar cells: Effects of the molecular structures on their properties

The design strategy of acceptor materials matched with poly(3-hexylthiophene) (P3HT) is highly desired for the development of low-cost organic solar cells (OSCs). Herein, we introduced strong electron-donating central units and weak electron-withdrawing end groups to construct the acceptors with high HOMO and LUMO, modulated the molecular symmetry and conjugation length by changing the structures of central units, and synthesized six acceptor molecules, namely, TDTC-O2F, TTDTC-O2F, TTTDTC-O2F, TDTC-ThBr, TTDTC-ThBr and TTTDTC-ThBr. The high LUMO energy level of the acceptors endowed the P3HT based OSCs with relatively high Voc values. Molecular symmetry, conjugation length of central units and the terminal structure jointly affect the molecular crystallinity and miscibility of the blends. Owing to the proper film morphology, the P3HT:TTDTC-ThBr based devices achieved the champion power conversion efficiency of 6.15 %.

Multifunctional Interface Modification Enables Efficient and Stable HTL-Free Carbon-Electroded CsPbI2Br Perovskite Solar Cells.

In recent years, hole transport layer-free all-inorganic CsPbI2Br carbon-electroded perovskite solar cells (C-PSCs) have garnered significant attention due to a trade-off between stability and photovoltaic performance. However, there are inevitably many defects generated at the surfaces or grain boundaries of CsPbI2Br perovskite films, which will serve as carrier non-radiative recombination centers, and CsPbI2Br perovskite films are sensitive to water molecules to degrade, together with energy level mismatch between CsPbI2Br perovskite and carbon electrodes. Herein, 1-benzyl-3-methylimidazolium hexafluorophosphate (1-B-3-MIMPF6), an imidazolium-based ionic liquid simultaneously containing benzene ring and fluorine atoms, was introduced for the modification of the perovskite/carbon interface. The results showed that it could effectively reduce defects, enhance carrier transfer, mitigate carrier non-radiative recombination, facilitate energy alignment, and block moisture intrusion. Therefore, the photovoltaic performance of the modified PSCs with ITO/SnO2/CsPbI2Br/1-B-3-MIMPF6/carbon architecture has been boosted with a champion power conversion efficiency (PCE) of 13.47 %, open circuit voltage of 1.20 V, short circuit current density of 14.69 mA/cm2, and fill factor of 76 %. Moreover, the unencapsulated modified devices exhibited an improved stability and the PCE maintained 78 % of their initial PCE after 24 h storage at room temperature in a 30 %-35 % humidity environment, whereas that of the pristine devices dropped to almost zero.

Iodine Modulates the MACl‐Assisted Growth of FAPbI3 for High Efficiency Perovskite Solar Cells

AbstractThe preferential growth of α‐phase formamidinium perovskite (α‐FAPbI3) at low temperatures can be achieved with the incorporation of chloride‐based additives, with methylammonium chloride (MACl) being the most common example. However, compared to other less‐volatile chloride additives, MACl only remains in the growing perovskite film for a short time before evaporating during annealing, primarily influencing the early stages of film formation. In addition, evaporation of MACl as methylamine (MA0) and HCl can introduce a side reaction between MA0 and formamidinium (FA), undermining the compositional purity and phase stability of α‐FAPbI3. In this study, it is demonstrated that addition of iodine (I2) into the FAPbI3 precursor solution containing MACl suppresses the MA‐FA side reaction during annealing. Additionally, MACl evaporation is delayed owing to strong interaction with triiodide. The added I2 facilitates spontaneous growth of α‐FAPbI3 prior to annealing, with an improved bottom morphology due to the formation of fewer byproducts. Perovskite solar cells derived from an I2‐incorporated solution deliver a champion power conversion efficiency of 25.2% that is attributed to suppressed non‐radiative recombination.

Ruddlesden-Popper Perovskite Nanocrystals as Interface Modification Layer for Efficient Perovskite Solar Cells.

Perovskite nanocrystals are advantageous for interfacial passivation of perovskite solar cells (PSCs), but the insulating long alkyl chain surface ligands impede the charge transfer, while the conventional ligand exchange would possibly introduce surface defects to the nanocrystals. In this work, we reported novel in situ modification of CsPbBr3 nanocrystals using a short chain conjugated molecule 2-methoxyphenylethylammonium iodide (2-MeO-PEAI) for interfacial passivation of PSCs. Transmission electron microscopy studies with atomic resolution unveil the transformation from cubic CsPbBr3 to Ruddlesden-Popper phase (RPP) nanocrystals due to halogen exchange. Synergic passivation by the RPP nanocrystals and 2-MeO-PEA+ has led to suppressed interface defects and enhanced charge carrier transport. Consequently, PSCs with in situ modified RPP nanocrystals achieved a champion power conversion efficiency of 24.39%, along with an improvement in stability. This work brings insights into the microstructural evolution of perovskite nanocrystals, providing a novel and feasible approach for interfacial passivation of PSCs.

Defect Modulation via SnX2 Additives in FASnI3 Perovskite Solar Cells.

Tin halide perovskites suffer from high defect densities compared with their lead counterparts. To decrease defect densities, SnF2 is commonly used as an additive in tin halide perovskites. Herein, we investigate how SnF2 compares to other SnX2 additives (X = F, Cl, Br) in terms of electronic and ionic defect properties in FASnI3. We find that FASnI3 films with SnF2 show the lowest Urbach energies (EU) of 19 meV and a decreased p-type character, as probed with ultraviolet photoemission spectroscopy. The activation energy of ion migration, as probed with thermal admittance spectroscopy, for FASnI3 with SnF2 is 1.33 eV, which is higher than with SnCl2 and SnBr2, which are 1.22 and 0.79 eV, respectively, resulting in less ion migration. Because of improved defect passivation, the champion power conversion efficiency of FASnI3 with SnF2 is 7.47% and only 1.84% and 1.20% with SnCl2 and SnBr2, respectively.