Sn-based Perovskite Solar Cells Research Articles

Comprehensive study on phase stability of lead-free Sn-based perovskite FAxMA1-xSnI3

Perovskite solar cells have become the most important devices for solar power to electricity conversion. However, currently, high-efficiency perovskite solar cells still rely on the use of Pb, which is harmful to the environment. Seeking environmentally friendly perovskite solar cells is imperative, and Sn is the most effective substitute for Pb. However, Sn-based perovskites face challenges due to their brief lifespan and rapid degradation, underscoring the need to improve their phase stability - a problem with still unclear mechanisms. This study addresses this by adjusting the ratio of formamidinium to methylammonium (FA/MA) in FAxMA1-xSnI3, experimentally finding optimal stability in phase composition and photoluminescence intensity at a ratio where x = 0.75. Using Density Functional Theory (DFT) and a pre-trained, fine-tuned machine-learning model, we explore the favorable molecular structures and configurations within FAxMA1-xSnI3. We discover that the FA0.75MA0.25SnI3 composition exhibits the lowest valence band maximum, indicating minimal oxidation tendency. Further DFT calculations of mixing and formation energies confirm that this composition is the most stable, aligning well with experimental observations and elucidating the underlying mechanisms of phase stability in Sn-based perovskite solar cells.

Molecularly Engineered Alicyclic Organic Spacers for 2D/3D Hybrid Tin-based Perovskite Solar Cells.

The high defect density and inferior crystallinity remain great hurdles for developing highly efficient and stable Sn-based perovskite solar cells (PSCs). 2D/3D heterostructures show strong potential to overcome these bottlenecks; however, a limited diversity of organic spacers has hindered further improvement. Herein, a novel alicyclic organic spacer, morpholinium iodide (MPI), is reported for developing structurally stabilized 2D/3D perovskite. Introducing a secondary ammonium and ether group to alicyclic spacers in 2D perovskite enhances its rigidity, which leads to increased hydrogen bonding and intermolecular interaction within 2D perovskite. These strengthened interactions facilitate the formation of highly oriented 2D/3D perovskite with low structural disorder, which leads to effective passivation of Sn and I defects. Consequently, the MP-based PSCs achieved a power conversion efficiency (PCE) of 12.04% with superior operational and oxidative stability. This work presents new insight into the design of organic spacers for highly efficient and stable Sn-based PSCs.

Ternary Passivation for Enhanced Carrier Transport and Recombination Suppression in Highly Efficient Sn-Based Perovskite Solar Cells.

The exploration of nontoxic Sn-based perovskites as a viable alternative to their toxic Pb-based counterparts has garnered increased attention. However, the power conversion efficiency of Sn-based perovskite solar cells lags significantly behind their Pb-based counterparts. This study presents a ternary passivation strategy aimed at enhancing device performance, employing [6,6]-phenyl-C61-butyric-acid-methyl-ester (PCBM), poly(3-hexylthiophene) (P3HT), and indene C60 bisadduct (ICBA). These components play crucial roles in managing energy levels and enhancing carrier transportation, respectively. The results reveal that the introduction of the ternary system leads to improvements in carrier collection and transportation, accompanied by a suppression of the recombination process. Ultimately, the champion device achieves a remarkable performance with an efficiency of 14.64%. Notably, the device also exhibits robust operational and long-term stored stability.

Comparison of Pb-based and Sn-based perovskite solar cells using SCAPS simulation: optimal efficiency of eco-friendly CsSnI3 devices.

In this study, we employed the one-dimensional solar cell capacitance simulator (SCAPS-1D) software to optimize the performance of Pb-based and Sn-based (Pb-free) all-inorganic perovskites (AIPs) and organic-inorganic perovskites (OIPs) in perovskite solar cell (PSC) structures. Due to the higher stability of AIPs, the performance of PSCs incorporating Cs-based perovskites was compared with that of FA-based perovskites, which are more stable than their MA-based counterparts. The impact of AIPs such as CsPbCl3, CsPbBr3, CsPbI3, CsSnCl3, CsSnBr3, and CsSnI3, as well as including FAPbCl3, FAPbBr3, FAPbI3, FASnCl3, FASnBr3, and FASnI3, was investigated. SnO2 and Cu2O were selected as an inorganic electron transport layer (ETL) and a hole transport layer (HTL), respectively. CsSnBr₃, CsSnI₃, FASnCl₃, and FASnBr₃ exhibited higher efficiency compared to their Pb-based counterparts. Additionally, most Cs-based perovskites, excluding CsPbI₃, demonstrated better performance relative to their FA counterparts. CsSnI3 AIP device also shows the highest short circuit current density (JSC) of 32.85mA/cm2, the best power conversion efficiency (PCE) of 16.00%, and the least recombination at the SnO2/CsSnI3 interface. The thickness, doping, and total defect density of CsSnI3 PSC have been systematically investigated and optimized to obtain the PCE of 17.36%. These findings highlight the potential of CsSnI3 PSCs as efficient and environmentally friendly PSCs.

Thickness-derived optical-electrical management in Sn-based perovskite solar cells

Tin-based perovskite solar cells (TPSCs) have attracted great attention due to their promising photovoltaic performance and environmental friendliness. Adequate photon trapping and efficient carrier utilization are known to be the keys to achieving high-performance devices, which are closely related to the thickness of the light-absorbing layer and the quality of film formation, respectively. Due to the ultra-fast crystallization characteristics and low defect formation energy, thick tin-based perovskite films are faced with poor electrical performance due to poor quality. Thin tin-based perovskite films are easy to achieve low defects and high crystallization quality, but insufficient thickness leads to the problem of insufficient light trapping. To address these issues, we have thoroughly investigated the various aspects of the photoelectric conversion process in TPSC devices and, for the first time, explored the behavior of front-end optical field management. It is found that the self-constructed microcavity effect can effectively improve the light trapping efficiency under the premise that a thin light-absorbing layer is used, so that sufficient photon trapping and excellent carrier transport characteristics can be ensured simultaneously to realize a high-performance device. Different from the traditional film formation and defect modulation strategy, the present work provides a feasible idea for the performance enhancement of TPSC devices, and is also of great significance for cost control and environmental protection issues in commercial applications.

Minimization of Energy Level Mismatch of PCBM and Surface Passivation for Highly Stable Sn-Based Perovskite Solar Cells by Doping n-Type Polymer.

Developing high-performance and stable Sn-based perovskite solar cells (PSCs) is difficult due to the inherent tendency of Sn2+ oxidation and, the huge energy mismatch between perovskite and Phenyl-C61-butyric acid methyl ester (PCBM), a frequently employed electron transport layer (ETL). This study demonstrates that perovskite surface defects can be passivated and PCBM's electrical properties improved by doping n-type polymer N2200 into PCBM. The doping of PCBM with N2200 results in enhanced band alignment and improved electrical properties of PCBM. The presence of electron-donating atoms such as S, and O in N2200, effectively coordinates with free Sn2+ to prevent further oxidation. The doping of PCBM with N2200 offers a reduced conduction band offset (from 0.38 to 0.21eV) at the interface between the ETL and perovskite. As a result, the N2200 doped PCBM-based PSCs show an enhanced open circuit voltage of 0.79V with impressive power conversion efficiency (PCE) of 12.98% (certified PCE 11.95%). Significantly, the N2200 doped PCBM-based PSCs exhibited exceptional stability and retained above 90% of their initial PCE when subjected to continuous illumination at maximum power point tracking for 1000h under one sun.

Machine learning guided efficiency improvement for Sn-based perovskite solar cells with efficiency exceeding 20%

Machine learning guided efficiency improvement for Sn-based perovskite solar cells with efficiency exceeding 20%

Dion-Jacobson-Phase 2D Sn-Based Perovskite Comprising a High Dipole Moment of π-Conjugated Short-Chain Organic Spacers for High-Performance Solar Cell Applications.

The stability issue of Sn-based perovskite solar cells (PSCs) is expected to be resolved by involving a two-dimensional (2D) layered structure. However, Sn-based 2D PSCs, especially Dion-Jacobson (DJ)-phase ones with potentially good stability, have rarely been reported. Herein, superior DJ-phase Sn 2D perovskites with 3-aminobenzylamine (3ABA2+) or 4-aminobenzylamine (4ABA2+) π-conjugated short-chain ligands are reported to fabricate efficient 2D lead-free PSCs. Notably, the high dipole moment of the 3ABAI2 organic spacer is approved to possess faster charge transfer for forming (3ABA)FA4Sn5I16 2D perovskite with an extremely low exciton binding energy (only 84 meV). In combination with a diacetate partial substitution and methylamine iodide/bromide (MAI/MABr) post-treatment strategy to delay crystallization and improve compactness and coverage of the perovskite film, a record power conversion efficiency (PCE) of 6.81% and stability of 840 h (less than 5% degradation in a N2 atmosphere for unencapsulated devices) are acquired in eventual (3ABA)FA4Sn5I16 2D PSCs, which are among the highest PCE and the longest stability of Sn-based 2D PSCs reported to date. Our work provides a prospective molecule design and film preparation strategy of 2D Sn perovskites toward nontoxic high-performance tin-based PSCs, which pushes the almost stagnant research forward.

Synergistic Modulation of Sn-Based Perovskite Solar Cells with Crystallization and Interface Engineering.

A high-quality Sn-based perovskite absorption layer and effective carrier transport are the basis for high-performance Sn-based perovskite solar cells. The suppression of Sn2+ oxidation and rapid crystallization is the key to obtaining high-quality Sn-based perovskite film. And interface engineering is an effective strategy to enhance carrier extraction and transport. In this work, tin fluoride (SnF2) was introduced to the perovskite precursor solution, which can effectively modulate the crystallization and morphology of Sn-based perovskite layer. Furthermore, the hole-transporting layer of PEDOT:PSS was modified with CsI to enhance the hole extraction and transport. As a result, the fabricated inverted Sn-based perovskite solar cells demonstrated a power conversion efficiency of 7.53% with enhanced stability.

Charge-Transfer States at the Fullerene Interface Cause Nonradiative Recombination Losses in Sn-Based Perovskite Solar Cells

Charge-Transfer States at the Fullerene Interface Cause Nonradiative Recombination Losses in Sn-Based Perovskite Solar Cells

High Performance and Efficiency Recovery in Sn‐Based Flexible Perovskite Solar Cells by Antioxidant Vanillin and Microwave Treatment

AbstractPerovskite based on Sn have attracted extensive attention to address the toxicity challenge associated with Pb‐based perovskite solar cells. However, Sn‐based perovskite solar cells（SPSCs）are notable for their poor stability and loss of efficiency due to rapid oxidation of Sn2+ to Sn4+ in air. To slow down the rapid oxidation, a number of antioxidants are suggested. Nevertheless, the antioxidant normally gets oxidized to non‐antioxidizing by‐products in a single‐stage redox reaction and loses the function of oxidation prevention. Herein, vanillin is introduced, a natural antioxidant with a double‐staged redox reaction to inhibit the oxidation of Sn2+ or reduce Sn4+ back to Sn2+, which improves the efficiency and prolongs the open‐air stability of SPSCs. With 7.5% vanillin doping, an outstanding efficiency of 13.18% is achieved. Moreover, exposure of the solar cell to 160 W microwave irradiation for 3 minutes resulted in significant efficiency recovery from 88% to 96.5% at 812 hours and from 35.7% to 65.4% after 2200 hours of aging. This work reveals the potential of natural antioxidation and short microwave irradiation as suitable approaches to elevate the efficiency and lifetime of SPSCs.

The Analysis of Defect Structure of Sn-based Perovskite Solar Cell Materials Using First-principles Calculations

The Analysis of Defect Structure of Sn-based Perovskite Solar Cell Materials Using First-principles Calculations

Data-driven design for enhanced efficiency of Sn-based perovskite solar cells using machine learning

In this study, a novel three-step learning-based machine learning (ML) methodology is developed utilizing 26 000 experimental records from The Perovskite Database Project. A comprehensive set of 29 features encompassing both categorical and numerical data was utilized to train various ML models for various solar cell performance metrics, including open-circuit voltage (VOC), short-circuit current (JSC), fill factor (FF), and power conversion efficiency (PCE). The model accuracy was assessed using four key metrics: mean absolute error, mean square error, root mean square error, and R2 score. Among the constructed models, random forest (RF) emerged as the standout performer, boasting an R2 score of 0.70 for PCE. This RF model was then used for prediction on the large, optimized design pool of Sn-based perovskite data with intent to probe a viable non-toxic substitute to the standard Pb-based absorber. A three-step algorithm was tailored, which led to the discovery of a new set of feature combinations, showcasing a PCE improvement over the existing peak performance of Sn-based devices. The key aspects identified were device architecture, dimensionality, and deposition procedures for essential layers, including the electron transport layer, the hole transport layer, the perovskite absorber layer, and the back-contact. Through consideration of these features, an impressive increase in PCE was achieved. There was a 28.35% increase in PCE from 12.24% to 15.71% for architecture optimization and a 24.6% increase in PCE from 12.24% to 15.25% for deposition method optimization. This study additionally addresses the effective implementation of target encoding applied to a diverse set of categorical feature labels. The data-driven methodology proposed in this study allows scientists to efficiently identify an optimal architecture and deposition parameters for non-toxic Sn-based perovskite materials with a much higher anticipated device PCE compared to traditional trial-and-error analyses. Further exploration and exploitation of the current investigation is expected to lead to successful and sustainable development of highly efficient Sn-based perovskite solar cells.

Synergetic Regulation of Interface Defects and Carriers Dynamics for High-Performance Lead-Free Perovskite Solar Cells.

Severe nonradiative recombination and open-circuit voltage loss triggered by high-density interface defects greatly restrict the continuous improvement of Sn-based perovskite solar cells (Sn-PVSCs). Herein, a novel amphoteric semiconductor, O-pivaloylhydroxylammonium trifluoromethanesulfonate (PHAAT), is developed to manage interface defects and carrier dynamics of Sn-PVSCs. The amphiphilic ionic modulators containing multiple Lewis-base functional groups can synergistically passivate anionic and cationic defects while coordinating with uncoordinated Sn2+ to compensate for surface charge and alleviate the Sn2+ oxidation. Especially, the sulfonate anions raise the energy barrier of surface oxidation, relieve lattice distortion, and inhibit nonradiative recombination by passivating Sn-related and I-related deep-level defects. Furthermore, the strong coupling between PHAAT and Sn perovskite induces the transition of the surface electronic state from p-type to n-type, thus creating an extra back-surface field to accelerate electron extraction. Consequently, the PHAAT-treated device exhibits a champion efficiency of 13.94% with negligible hysteresis. The device without any encapsulation maintains 94.7% of its initial PCE after 2000h of storage and 91.6% of its initial PCE after 1000h of continuous illumination. This work provides a reliable strategy to passivate interface defects and construct p-n homojunction to realize efficient and stable Sn-based perovskite photovoltaic devices.

Modelling of Germanium-Based Perovskite Solar Cell for Different Hole Transport Materials and Defect Density

The performance of four distinct materials (organic and inorganic) was simulated and analyzed as hole transport layer (HTL) in the design of germanium (Ge)-based Perovskite Solar Cell (PSC). A 1-dimensional numerical software (SCAPS 1-D) has been applied to simulate the HTL candidates: spiro-OMeTAD, PTAA, nickel oxide (NiO), and copper (I) thiocyanate (CuSCN), with tin (IV) dioxide (SnO2) as the electron transport layer (ETL). The thickness of the methylammonium germanium iodide (CH3NH3GeI3) absorber was varied from 300 nm to 1100 nm, and the highest simulated power conversion efficiency was achieved at a thickness of 800 nm for all HTL candidates. It was observed that the inorganic CuSCN outperformed its counterparts with a power conversion efficiency (PCE) of 25.38%. The effect of the perovskite absorber’s defect density was investigated, and ultimately, it was demonstrated that this value is disproportionately related to the PCE. A reduction of nearly 98% in PCE was recorded when the defect density increased from 1x1014 cm-3 to 1x1020 cm-3. Additionally, for a constant ETL thickness of 80 nm, it was revealed that the PCE would decrease slightly, ranging from 0.1% to 0.3%, with an increase in HTL thickness from 50 nm to 300 nm. Comparing the PCE of our current work with published reports further justifies its competitiveness. Full Text: PDF References W.R. Becquerel, "Becquerel Photovoltaic Effect in Binary Compounds", J. Chem. Phys. 32, 1505 (1960). CrossRef A. Kojima, K. Teshima, Y. Shirai, T. Miyasaka, "Organometal Halide Perovskites as Visible-Light Sensitizers for Photovoltaic Cells", J. Am. Chem. Soc. 131, 6050 (2009). CrossRef M.M. Salah, K.M. Hassan, M. Abouelatta, A. Shaker, "A comparative study of different ETMs in perovskite solar cell with inorganic copper iodide as HTM", Optik 178, 958 (2019). CrossRef S. Rai, B. Pandey, A. Garg, D. Dwivedi, "Hole transporting layer optimization for an efficient lead-free double perovskite solar cell by numerical simulation", Opt. Mater, 121, 111645 (2021). CrossRef H. Liangsheng, Z. Min, S. Yubao, M. Xinxia, W. Jiang, Z. Qunzhi, F, Zaiguo, L. Yihao, H. Guoyu, L. Tong, "Tin-based perovskite solar cells: Further improve the performance of the electron transport layer-free structure by device simulation", Sol. Energy, 230, 345 (2021). CrossRef K. Fatema, M. Arefin, "Enhancing the efficiency of Pb-based and Sn-based perovskite solar cell by applying different ETL and HTL using SCAPS-ID", Opt. Mater. 125, 112036 (2022). CrossRef P. Patel, "Device simulation of highly efficient eco-friendly CH3NH3SnI3 perovskite solar cell", Sci. Rep., 11, 3082 (2021). CrossRef P. Roy, Y. Raoui, A. Khare, "Design and simulation of efficient tin based perovskite solar cells through optimization of selective layers: Theoretical insights", Opt. Mater., 125, 112057 (2022). CrossRef A.I. Azmi, M.Y. Mohd Noor, M.H.I. Ibrahim, F. Ahmad, M.H. Ibrahim, "A Numerical Simulation of Transport Layer Thickness Effect in Tin-Based Perovskite Solar Cell", JJEE, 8, 355 (2022). CrossRef A.A. Kanoun, M.B. Kanoun, A.E. Merad, S. Goumri-Said, "Toward development of high-performance perovskite solar cells based on CH3NH3GeI3 using computational approach", Sol. Energy, 182, 237 (2019). CrossRef A. Hima, N. Lakhdar, "Enhancement of efficiency and stability of CH3NH3GeI3 solar cells with CuSbS2", Opt. Mater., 99, 109607 (2020). CrossRef S.T. Jan, M. Noman, "Influence of layer thickness, defect density, doping concentration, interface defects, work function, working temperature and reflecting coating on lead-free perovskite solar cell", Sol. Energy, 237, 29 (2022). CrossRef

Anchoring self-assembled monolayer at perovskite/hole collector interface for wide bandgap Sn-based solar cells with a record efficiency over 12%

In perovskite solar cells (PSCs), surface and interfacial conditions play a crucial role in determining overall device performance. In typical p-i-n architecture of wide bandgap (WBG, 1.6–1.8 eV) Sn-based PSCs, the interface between hole transport layer (HTL) and perovskite (PVK) has a significant impact on hole transport, interfacial chemical interactions, and perovskite film quality. This study aims to address these issues by incorporating self-assembled monolayers (SAMs) MeO-2PACz and 2PACz at the PEDOT:PSS HTL/Sn-PVK interface. X-ray photoelectron spectroscopy confirmed the interaction between the anchoring group (P-O−) of the SAM and S+ in PEDOT:PSS through phosphonic acid deprotonation at the interface, and improved work function was observed through the UPS study. Furthermore, the SAMs contributed to the formation of a compact PVK film with enhanced preferential orientation. Interestingly, a chemical interaction between the oxygen-donor of the methoxy (CH3O−) terminal group in MeO-2PACz and the Sn-halide octahedra was observed, which partly contributed to suppress the oxidation of Sn2+ state and defect density of perovskite. Additionally, femtosecond transient absorption spectroscopy (fs-TAS) showed faster trap filling (τ1) characteristics (τ1∼19 ps). Fs-TAS and photoluminescence further indicated fast hole extraction (τ2∼125 ps) as well as high quenching efficiency of 47%. Based on these findings, an unprecedented efficiency of η∼12.16% (certified 11.60%) was achieved in WBG Sn-PSCs using the HTL/MeO-2PACz/PVK structure, outperforming the HTL/2PACz/PVK (8.78%) and HTL/PVK (7.44%) structures. This study provides crucial guidelines on interfacial engineering for WBG Sn-PSCs.

Optimization of Sn-based perovskite solar cells with the antisolvent doped by acetaldoxime

Optimization of Sn-based perovskite solar cells with the antisolvent doped by acetaldoxime

The potassium acetate additive enhances the stability of the FA0.75MA0.25SnI3 precursor solution and the performance of corresponding perovskite solar cells

Although Sn-based perovskite solar cells (PSCs) have achieved excellent conversion efficiency, the issue of easy oxidation of Sn2+ still needs to be addressed. This paper believes that the antioxidant ability of PSCs can be improved starting from the precursor solutions. In this work, potassium acetate (KAc) is first added to FA0.75MA0.25SnI3 precursor solution to suppress the oxidation of Sn2+ and to prepare a high-quality KAc-FA0.75MA0.25SnI3 composite film. The KAc-FA0.75MA0.25SnI3 film has better crystallinity and optical absorption, reduced defect density and unnecessary non-radiative recombination while suppressing Sn2+ oxidation. Finally, the PSCs based on KAc-FA0.75MA0.25SnI3 film achieved an excellent power conversion efficiency of 9.62% and a long-term stability of over 850 h to retain 80% of its initial efficiency.

14.31 % Power Conversion Efficiency of Sn-Based Perovskite Solar Cells via Efficient Reduction of Sn4.

The photoelectric properties of nontoxic Sn-based perovskite make it a promising alternative to toxic Pb-based perovskite. It has superior photovoltaic performance in comparison to other Pb-free counterparts. The facile oxidation of Sn2+ to Sn4+ presents a notable obstacle in the advancement of perovskite solar cells that utilize Sn, as it adversely affects their stability and performance. The study revealed the presence of a Sn4+ concentration on both the upper and lower surfaces of the perovskite layer. This discovery led to the adoption of a bi-interface optimization approach. A thin layer of Sn metal was inserted at the two surfaces of the perovskite layer. The implementation of this intervention yielded a significant decrease in the levels of Sn4+ and trap densities. The power conversion efficiency of the device was achieved at 14.31 % through the optimization of carrier transportation. The device exhibited operational and long-term stability.

Metal oxide nanoparticles as an electron-transport layer in perovskite solar cell

The research on the application of lead-free perovskite materials as an active layer in solar cells has been positively carried out for the last few years. Although the efficiency of lead-contained metal halide-based Perovskite has reached above 25%, but lead is a highly toxic substance that is hazardous to the environment, and this is one of the obstacles to their commercialization. In this article, a Sn-based Perovskite (CH3NH3SnI3) solar cell with two distinct electron transport layers was simulated using GPVDM (General Purpose Photovoltaic Device Model) and fabricated with a simple sol-gel method. Along with the absorber layer, the charge transport materials also play an essential role in extracting electrical power. The comparison of ZnO and TiO2 as electron collectors has been investigated and characterized, the hole-carrying layer has been eliminated for better findings. Remarkably, we achieve an efficiency of 7.33% and 6.75% in simulation and 6.90% and 5.81% from fabricated devices using ZnO and TiO2, respectively.