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Transparent conductive oxide (TCO)‐coated glasses are the most expensive and environmentally impacting components of perovskite solar cells (PSCs), comprising 56% of the total cost of a perovskite module and 96% of its carbon footprint. Thus, recycling TCO glasses from end‐of‐life perovskite modules can reduce both their levelized cost of electricity and energy payback time. In this work, tin oxide (SnO2)‐coated indium tin oxide glasses are refurbished from n‐i‐p PSCs employing dimethyl sulfoxide as a green solvent to dissolve the upper layers of the devices. Employing the recovered substrates, new‐generation PSCs are produced, which retain the same champion power conversion efficiency (PCE) of 22.6% as fresh samples and display an even higher average PCE. This performance enhancement is investigated through compositional and electrical analyses that demonstrate that the proposed recycling protocol induces beneficial surface modifications on the SnO2/perovskite interface and trap passivation, boosting charge extraction. [ABSTRACT FROM AUTHOR]

Defect passivation is nowadays considered a must‐have route for high‐efficiency perovskite solar cells. However, a general rule that correlates the choice of passivating agents with performance enhancements is still missing. Herein, two different thiophene salts that are used as passivating agents are compared, namely thiophene methylammonium chloride and thiophene ethylammonium chloride (TEACl), which are used for the passivation of bulk and surface defects in triple‐cation‐based metal halide perovskites. First, it is observed that the surface passivation method leads to better device performances reaching a power conversion efficiency of 23.56%, with reduced voltage losses and increased fill factor when compared with the reference. Second, it is demonstrated that the chemical structure of the cation dictates its capability either in passivating bulk defects effectively or to form a superficial two‐dimensional/three‐dimensional heterostructure, which happens only for the TEACl case. The chemical composition and the cation dimension are responsible for device performance enhancement as observed by a joint spectroscopic and density functional theory simulations study, providing rational guidelines for further smart device design. [ABSTRACT FROM AUTHOR]

Defect‐mediated recombination losses limit the open‐circuit voltage (VOC) of perovskite solar cells (PSCs), negatively affecting the device's performance. Bulk and dimensional engineering have both been reported as promising strategies to passivate shallow defects, thus improving the photovoltaic conversion efficiency (PCE). Here, a combined bulk and surface treatment employing chlorine‐based compounds is employed. Methylammonium chloride (MACl) is used as a bulk additive, while 4‐methylphenethylammonium chloride (MePEACl) is deposited onto the perovskite surface to produce a low‐dimensional perovskite (LDP) and reduce nonradiative recombination. Through structural and morphological investigations, it can be confirmed that bulk and surface doping have a beneficial effect on the film morphology and its overall quality, while electroluminescence (EL) and photoluminescence (PL) analyses demonstrate an increased and more homogeneous emission. Applying this double passivation strategy in PSC fabrication, a boost is observed in both the short‐circuit current density and the VOC of the devices, achieving a champion 21.4% PCE while improving device stability. [ABSTRACT FROM AUTHOR]

Improving the perovskite/electron-transporting layer (ETL) interface is a crucial task to boost the performance of perovskite solar cells (PSCs). This is utterly fundamental in an inverted (p-i-n) configuration using fullerene-based ETLs. Here, we propose a scalable strategy to improve fullerene-based ETLs by incorporating high-quality few-layer graphene flakes (GFs), industrially produced through wet-jet milling exfoliation of graphite, into phenyl-C61-butyric acid methyl ester (PCBM). Our new composite ETL (GF:PCBM) can be processed into an ultrathin (∼10 nm), pinhole-free film atop the perovskite. We find that the presence of GFs in the PCBM matrix reduces defect-mediated recombination, while creating preferential paths for the extraction of electrons towards the current collector. The use of our GF-based composite ETL resulted in a significant enhancement in the open circuit voltage and fill factor of triple cation-based inverted PSCs, boosting the power conversion efficiency from ∼19% up to 20.8% upon the incorporation of GFs into the ETL., Competing Interests: There are no conflicts to declare., (This journal is © The Royal Society of Chemistry.)