Jing Li

Perovskite photovoltaics are limited by structural instabilities initiated during crystallization and amplified under operation. We report that a lattice-matched Prussian blue scaffold directs heterogeneous nucleation to produce highly oriented, strain-relaxed films. Its redox-active Fe–C≡N–Fe network mediates the conversion of Pb ⁰ and I ⁰ defects, and its rigid open framework suppresses A-site cation redistribution and the resulting electronic inhomogeneity under bias. This strategy yielded champion power conversion efficiencies of 26.1% (n-i-p) and 26.9% (p-i-n; 26.2% certified), scaling to 23.4% in 6-centimeter–by–6-centimeter minimodules and a certified 22.9% in 30-centimeter–by–30-centimeter submodules. Submodules with initial power conversion efficiencies ranging from 20.2 to 21.0% showed robust durability under accelerated aging and no discernible decline relative to a silicon reference over 5 months of outdoor testing.

Closing the gap between lab‐scale efficiency and module‐scale reliability is critical for the commercialization of perovskite photovoltaics. However, scaling up aggravates spatial heterogeneity, interfacial energetic disorder, and thermomechanical degradation, particularly at vacuum‐deposited oxide/perovskite junctions. Here, we report an all‐vacuum engineering strategy for SnO ₂ ‐based buried interfaces that addresses both optoelectronic and thermomechanical losses in scalable perovskite photovoltaics. In situ Eu co‐sputtering within a magnetron‐sputtered SnO ₂ framework regulates oxygen‐vacancy chemistry and homogenizes the interfacial energetic landscape, thereby promoting more efficient electron extraction. Building on this, bifacial modules achieve power conversion efficiencies of 17.85% at the 6 × 6 cm ² scale and 17.39% at a 175 cm ² aperture area, while the 6 × 6 cm ² modules retain 90.2% of their initial efficiency after 2000 h of maximum‐power‐point tracking under ISOS‐L‐3 conditions. Opaque devices with Au top electrodes further reach 19.89%, supporting the effectiveness of this buried‐interface strategy across different electrode configurations. After further introducing an evaporated ultrathin KCl interlayer, the initial efficiency is largely preserved, while buried interfacial strain under thermal stress is relieved and thermal‐cycling durability is improved, with 88.9% retention after 200 ISOS‐LT‐3 cycles. This work establishes all‐vacuum buried‐interface engineering as a practical route toward scalable and thermally stable perovskite photovoltaics.

Despite substantial improvements in the quality of perovskite films achieved through processing optimization, the prevalence of surface and interfacial defects underscores the critical need for efficient post-treatment strategies. Here, we report an expectable surface engineering approach using thermotropic liquid molecule 1-boc-piperazine (1-BP). The 1-BP undergoes a solid-to-liquid phase transition and spontaneously migrates to perovskite grain boundaries during annealing process, forming an active encapsulation layer that reconstructs the perovskite interface. The most attractive achievement of ion migration suppression by 1-BP has been evidentially revealed by the in-situ time-of-flight secondary ion mass spectrometry. Base on the approach, the n-i-p perovskite solar cells achieve a certified power conversion efficiency of 25.62%, with perovskite solar modules achieving PCE of 22.03% (active area: 22.8 cm²). Furthermore, the 1-BP engineered devices demonstrated exceptional stability, retaining T₉₀ after 1500 h at 65 °C with continuous illumination and T₈₇ after 1000 h at 85 °C/85% RH.

Currently, perovskite solar cells have achieved commendable progresses in power conversion efficiency (PCE) and operational stability. However, some conventional laboratory-scale fabrication methods become challenging when scaling up material syntheses or device production. Particularly, the prolonged high-temperature annealing process for the crystallization of perovskites requires a substantial amount of energy consumption and impact the modules’ throughput. Here, we report a modified near-infrared annealing (NIRA) process, which involves the excess PbI₂ engineered crystallization, efficiently reduces the preparation time for perovskite active layer to within 20 s compared to dozens of min in conventional hot plate annealing (HPA) process. The study showed that the incorporated PbI₂ promoted the consistent nucleation of the perovskite film, leading to the subsequent rapid and homogeneous crystallization at the NIRA stage. Thus, highly crystalized perovskite film was realized with even better crystallization performance than conventional HPA-based film. Ultimately, efficient perovskite solar modules of 36 and 100 cm² were readily fabricated with the optimal PCEs of 22.03% and 20.18%, respectively. This study demonstrates, for the first time, the successful achievement of homogeneous and high-quality crystallization in large-area perovskite films through rapid NIRA processing. This approach not only significantly reduces energy consumption during production, but also substantially shortens the manufacturing cycle, paving a new path toward the commercial-scale application of perovskite solar modules.

Ligand-tailored synthesis of homogeneous NiO _x nanocrystals enables eco-friendly and scalable fabrication of high-performance n–i–p perovskite solar cells.

Li‐TFSI doped spiro‐OMeTAD is widely recognized as a beneficial hole transport layer (HTL) in perovskite solar cells (PSCs), contributing to high device efficiencies. However, the uncontrolled migration of lithium ions (Li⁺) during device operation has impeded its broad adoption in scalable and stable photovoltaic modules. Herein, an additive strategy is proposed by employing ferrocenium hexafluorophosphate (FcPF₆) as a relay medium to enhance the hole extraction capability of the spiro‐OMeTAD via the instant oxidation function. Besides, the novel Fc–Li interaction effectively restricts the movement of Li⁺. Simultaneously, the dissociative hexafluorophosphate group is cleverly exploited to regulate the unstable iodide species on the perovskite surface, further inhibiting the formation of migration channels and stabilizing the interfaces. This modification leads to power conversion efficiencies (PCEs) reaching 22.13% and 20.27% in 36 cm² (active area of 18 cm²) and 100 cm² (active area of 56 cm²) perovskite solar modules (PSMs), respectively, with exceptional operational stability obtained for over 1000 h under the ISOS‐L‐1 procedure. The novel FcPF₆‐based engineering approach is pivotal for advancing the industrialization of PSCs, particularly those relying on high‐performance spiro‐OMeTAD‐ based HTLs.

Metal halide perovskite materials inherently possess imperfections, particularly under nonequilibrium conditions, such as exposure to light or heat. To tackle this challenge, we introduced stearate ligand-capped nickel oxide (NiO_x), a redox-sensitive metal oxide with variable valence, into perovskite intermediate films. The integration of NiO_x improved the efficiency and stability of perovskite solar cells (PSCs) by offering multifunctional roles: (1) chemical passivation for ongoing defect repair, (2) energetic passivation to bolster defect tolerance, and (3) field-effect passivation to mitigate charge accumulation. Employing a synergistic approach that tailored these three passivation mechanisms led to a substantial increase in the devices' efficiencies. The target cell (0.12 cm²) and module (18 cm²) exhibited efficiencies of 24.0 and 22.9%, respectively. Notably, the encapsulated modules maintained almost 100 and 87% of the initial efficiencies after operating for 1100 h at the maximum power point (60 °C, 50% RH) and 2000 h of damp-heat testing (85 °C, 85% RH), respectively. Outdoor real-time tests further validated the commercial viability of the NiO_x-assisted PSMs. The proposed passivation strategy provides a practical and uncomplicated approach for fabricating high-efficiency and stable photovoltaics.