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Mixed lead‐tinv halide (LTH) perovskite solar cells (LTH‐PSCs) can reduce the toxicity concerns of full lead‐based PSCs and potentially optimize the bandgap to maximize efficiency. However, commonly used hole‐transporting material (HTM) 2,2′,7,7′‐tetrakis(N,N‐di‐p‐methoxyphenyl‐amine)9,9′‐spirobifluorene (Spiro‐OMeTAD) with additional dopants Li‐bis(trifluoromethanesulfonyl) imide (Li‐TFSI) and 4‐tert‐butylpyridine (t‐BP) deteriorate oxidation Sn2+ to Sn4+ leading to trap formation. Here, the study introduces a novelty Sn‐friendly HTM for Sn‐rich LTH‐PSCs, combining Spiro‐OMeTAD with 4‐Isopropyl‐4′‐methyldiphenyliodonium tetrakis(pentafluorophenyl)borate (dpi‐TPFB) as a dopant and blended with poly(3‐hexylthiophene‐2,3‐diyl) (P3HT). This blended HTM avoids the harmful effects of Li‐TFSI and t‐BP dopants and leverages the beneficial hydrophobic properties of P3HT, which predominantly resides on the surface with a face‐on orientation. This arrangement not only enhances charge transport and extraction but also improves device stability by protecting the perovskite from environmental factors. Optimizing the P3HT concentration of blended HTM achieved a PCE of 17.27%, the highest reported for n‐i‐p structured Sn‐rich mixed LTH‐PSCs. This HTM also significantly improved device stability, maintaining over 90% of the initial PCE after 3000 h of storage and 80% under maximum power point tracking (MPPT) for 550 h in the air. [ABSTRACT FROM AUTHOR]

Alkyl‐primary‐ammonium‐based room‐temperature ionic liquids (RTILs) designed to exhibit specific reactivities allowing functions that cannot be achieved by other RTILs have recently emerged. The archetype of the reactive RTILs is n‐octylammonium bis(trifluoromethanesulfonyl)imide (OA‐TFSI), which has promising functions as an additive for hole transport materials (HTMs) in perovskite solar cells (PSCs); the high reactivity of the OA cations on the perovskite surface allows spontaneous perovskite passivation via HTM deposition, effectively improving the photovoltaic (PV) performance. However, although the reactivity manipulation of the reactive RTILs is instrumental for exploiting their potential functions and exploring their application scope, methods for reactivity control have not been developed. Herein, it is proposed that the coaddition of a pyridine derivative (4‐tert‐butylpridine: TBP) can effectively manipulate the reactivity of OA‐TFSI by controlling the protonation between OA and the 2,2′,7,7′‐tetrakis‐(N,N‐di‐4‐methoxyphenylamino)‐9,9′‐spirobifluorene (Spiro‐OMeTAD) HTM. The TBP prevents OA deprotonation presumably via stabilization of the OA cation, thus retaining its ammonium form, which allows efficient spontaneous perovskite passivation, effectively enhancing the PV performance. This reveals the protonation preference in the OA‐TFSI system, which is opposite to that in conventional RTILs. This first proposal of a method in manipulating reactivity of the reactive RTILs will contribute to the development of materials science. [ABSTRACT FROM AUTHOR]

Electron donor (D)-electron acceptor (A) type conjugated polymers present bright prospects as dopant-free hole-transporting materials (HTMs) for perovskite solar cells (PVSCs). Most of the reported D-A polymeric HTMs contain equivalent amounts of D and A units, while the appropriate excess proportion of D units could optimize the aggregation state of polymer chains and improve the hole transport properties of the polymers. Herein, a non-equivalent D-A copolymerization strategy was utilized to develop three indacenodithiophene-benzotriazole-based polymeric HTMs for PVSCs, named as F-10, F-15, and F-20, and the equivalent D-A polymer F-00 was studied in parallel. Effects of D:A ratio on the hole transport properties of these D-A type polymeric HTMs, including energy level, molecular stacking, hole mobility, and surface morphology, were investigated by theoretical simulation and test analysis. F-15 performed best due to the appropriate D:A ratio, endowing the PVSCs a champion power conversion efficiency of 20.37% with high stability, which confirms the fine-tuning D:A ratio via non-equivalent D-A copolymerization strategy is very helpful to construct D-A type polymeric HTMs for highperformance PVSCs. [ABSTRACT FROM AUTHOR]

Perovskite solar cells (PSCs) offer advantages over widely deployed silicon solar cells in terms of ease of fabrication; however, the device is still under rigorous materials optimization for cell performance, stability, and cost. In this work, we explore a version of a PSC by replacing the polymeric hole transport layer (HTL) such as Spiro-OMeTAD, P3HT, and PEDOT: PSS with a more air-stable metal oxide, viz., nitrogen-doped titanium dioxide (TiO2:N). Numerical simulations on formamidinium (FA)-based PSCs in the FTO/TiO2/FAPbI3/Ag configuration have been carried out to depict the behaviour of the HTL as well as the effect of absorber layer thickness (∆t) on photovoltaic parameters. The results show that the cell output increases when the HTL bandgap increases from 2.5 to 3.0 eV. By optimizing the absorber layer thickness and the gradient in defect density (Nt), the device structure considered here can deliver a maximum power conversion efficiency of ~21.38% for a lower HTL bandgap (~2.5 eV) and ~26.99% for a higher HTL bandgap of ~3.0 eV. The results are validated by reproducing the performance of PSCs employing commonly used polymeric HTLs, viz. Spiro-OMeTAD, P3HT, and PEDOT: PSS as well as high power conversion efficiency in the highly crystalline perovskite layer. Therefore, the present study provides high-performing, cost-effective PSCs using TiO2:N. [ABSTRACT FROM AUTHOR]

Electron donor (D)-electron acceptor (A) type conjugated polymers present bright prospects as dopant-free hole-transporting materials (HTMs) for perovskite solar cells (PVSCs). Most of the reported D-A polymeric HTMs contain equivalent amounts of D and A units, while the appropriate excess proportion of D units could optimize the aggregation state of polymer chains and improve the hole transport properties of the polymers. Herein, a non-equivalent D-A copolymerization strategy was utilized to develop three indacenodithiophene-benzotriazole-based polymeric HTMs for PVSCs, named as F-10, F-15, and F-20, and the equivalent D-A polymer F-00 was studied in parallel. Effects of D : A ratio on the hole transport properties of these D-A type polymeric HTMs, including energy level, molecular stacking, hole mobility, and surface morphology, were investigated by theoretical simulation and test analysis. F-15 performed best due to the appropriate D : A ratio, endowing the PVSCs a champion power conversion efficiency of 20.37 % with high stability, which confirms the fine-tuning D : A ratio via non-equivalent D-A copolymerization strategy is very helpful to construct D-A type polymeric HTMs for high-performance PVSCs., (© 2024 Wiley-VCH GmbH.)

Perovskite solar cells (PSCs) offer advantages over widely deployed silicon solar cells in terms of ease of fabrication; however, the device is still under rigorous materials optimization for cell performance, stability, and cost. In this work, we explore a version of a PSC by replacing the polymeric hole transport layer (HTL) such as Spiro-OMeTAD, P3HT, and PEDOT: PSS with a more air-stable metal oxide, viz., nitrogen-doped titanium dioxide (TiO2:N). Numerical simulations on formamidinium (FA)-based PSCs in the FTO/TiO2/FAPbI3/Ag configuration have been carried out to depict the behaviour of the HTL as well as the effect of absorber layer thickness (∆t) on photovoltaic parameters. The results show that the cell output increases when the HTL bandgap increases from 2.5 to 3.0 eV. By optimizing the absorber layer thickness and the gradient in defect density (Nt), the device structure considered here can deliver a maximum power conversion efficiency of ~21.38% for a lower HTL bandgap (~2.5 eV) and ~26.99% for a higher HTL bandgap of ~3.0 eV. The results are validated by reproducing the performance of PSCs employing commonly used polymeric HTLs, viz. Spiro-OMeTAD, P3HT, and PEDOT: PSS as well as high power conversion efficiency in the highly crystalline perovskite layer. Therefore, the present study provides high-performing, cost-effective PSCs using TiO2:N.

Recently, perovskite solar cells (PSCs) basing on quasi-two-dimensional (quasi-2D) perovskites with hydrophobic bulky organic cations have received a lot of interests owing to their superior moisture stability. While quasi-2D perovskites have achieved great success in planar p-i-n PSCs, their application in planar n-i-p devices and the corresponding efficiencies lag far behind. In our work, (FPEA) 2 (MA) 4 Pb 5 I 16 perovskite films with high crystallinity, compact and smooth surface were deposited on electron transport layer with NH 4 SCN as an additive. Formamidinium (FA+) were then incorporated into the FPEA based perovskite films to partially replace methylammonium (MA+), and effects of FA+ on the film's vertical orientation, light absorption capacity, carrier lifetime, defect density and electron mobility were studied. It was found that when molar ratio of FA/MA = 0.5/9.5, the film had the highest vertical orientation, enhanced light absorption, less carrier recombination loss. The obtained (FPEA) 2 (FA 0.05 MA 0.95) 4 Pb 5 I 16 based n-i-p PSCs gave a maximum efficiency of 12.17% under standard illumination, retaining 83% of the initial efficiency after stored in air environment (25–30 °C) with 40 ± 5% RH for 1080 h. The results demonstrate an efficient approach to prepare high-quality quasi-2D perovskite films in a n-i-p structure as well as improved device efficiency and stability. [Display omitted] • Optimize the film quality of quasi-2D perovskites in n-i-p structured PSCs. • The FA+ doping is favour to guide better crystalinity and vertical orientation for quasi-2D perovskites. • The incorporation FA+ helps to suppress charge recombination loss and reduce band gap. • FA+ doped device maintains 83% of the initial PCE after being kept in a humidity of 40% for 1080 h. [ABSTRACT FROM AUTHOR]