Key Takeaways & Executive Findings
- •• • Phase-locked films maintained over 84% of initial photoluminescence intensity across all regions under identical aging conditions, whereas control devices exhibited only 34% efficiency retention at early-coated positions after thermal cycling, demonstrating that morphological homogeneity suppresses autocatalytic degradation pathways. • • Encapsulated modules retained over 90% of initial efficiency after 1500 h of 85°C maximum power point tracking in ambient air (ISOS-L-2 protocol) and after 2300 h under 85°C/85% RH damp-heat testing (ISOS-D-3 protocol), representing among the best stability benchmarks for large-area perovskite modules. • • The TMPU-based phase-locking strategy achieved a module efficiency of 21.5%, significantly surpassing the 20% threshold for scalable modules fabricated in ambient air, while maintaining compatibility with high-throughput blade-coating processes. • • The strategy uniquely addresses the kinetic and spatial dimensions of upscaling, linking crystallization kinetics with environmental robustness and large-area homogeneity, whereas previous approaches focused solely on thermodynamic stabilization or moisture-tolerant formulations.
Abstract
Organic-inorganic hybrid lead halide perovskites exhibit exceptional photovoltaic properties, yet their low crystallization energy promotes defect generation and necessitates precise control over synthesis parameters, hindering scalable fabrication. Ambient large-area coating methods suffer from environmental disturbances, leading to nonuniform crystallization and mixed α/δ phases, resulting in module efficiencies below 20% compared to >27% for lab-scale spin-coated cells. This work introduces a phase-locking strategy using 3-ureidopropyltrimethoxysilane (TMPU) incorporated into the PbI2 precursor solution during two-step blade coating. TMPU undergoes simultaneous cross-linking and interaction with the perovskite intermediate, forming a dynamically evolving intergranular network that blocks moisture and reduces the energy barrier for α-FAPbI3 formation. This approach achieves spatiotemporally homogeneous crystallization, eliminating directional inhomogeneity. Under segmented and monolithic aging protocols, control devices exhibited severe position-dependent degradation with only 34% efficiency retention at early-coated positions after thermal cycling, whereas phase-locked films maintained over 84% of initial photoluminescence intensity across all regions. Encapsulated modules retained over 90% of initial efficiency after 1500 h of 85°C maximum power point tracking (ISOS-L-2) and after 2300 h under 85°C/85% RH damp-heat testing (ISOS-D-3). The TMPU-based strategy combines exceptional performance (21.5% module efficiency) with robust stability, offering a distinct advantage over alternative approaches. This work addresses the kinetic and spatial dimensions of upscaling, demonstrating that morphological uniformity is a fundamental contributor to stability, marking a critical advance toward practical deployment of perovskite photovoltaics.
1. Introduction
Scalable manufacturing of perovskite photovoltaics has been fundamentally constrained by the trade-off between facile crystallization and defect generation. While laboratory-scale spin-coated cells achieve efficiencies exceeding 27%, large-area modules fabricated in ambient air via blade coating or similar methods have yet to surpass 20%. This gap stems from environmental disturbances—moisture, oxygen, temperature fluctuations, and spatial variations in solvent evaporation—that induce undesirable intermediate or mixed α/δ phases and spatially nonuniform crystallization. These nonuniformities not only degrade performance but also trigger self-amplifying degradation pathways, where early-coated regions with higher defect density and PbI2 accumulation act as catalytic centers, propagating decomposition across the film. Consequently, control devices exhibit severe position-dependent degradation, retaining only 34% of initial efficiency at early-coated positions after thermal cycling.
Existing strategies to address this challenge have focused on thermodynamic stabilization through intermediate-phase engineering or moisture-tolerant formulations, yet they fail to address the kinetic and spatial dimensions of upscaling. The TMPU-based phase-locking strategy introduced in this work directly tackles these bottlenecks by incorporating 3-ureidopropyltrimethoxysilane (TMPU) into the PbI2 precursor solution. During annealing, TMPU cross-links and interacts with the perovskite intermediate, forming a dynamically evolving intergranular network that blocks moisture intrusion and reduces the energy barrier for α-FAPbI3 formation. This dual action ensures spatiotemporally homogeneous crystallization, eliminating directional inhomogeneity and suppressing autocatalytic degradation. The result is a scalable process that achieves 21.5% module efficiency with exceptional stability—retaining over 90% of initial efficiency after 1500 h of 85°C MPPT and 2300 h of damp-heat testing—demonstrating that morphological uniformity is not merely a performance enhancer but a fundamental contributor to long-term operational reliability.
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Huang Xici, Zhang Qifeng, Cao Guozhong (2026). TMPU-Based Phase-Locking Strategy for Spatiotemporally Homogeneous Crystallization Enables Ambient Scalable Perovskite Photovoltaics. SCIENCE CHINA Materials. https://doi.org/10.1007/s40843-026-4463-3
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Frequently Asked Questions
What is the specific role of TMPU in achieving spatiotemporally homogeneous crystallization, and how does it interact with the perovskite intermediate during annealing?
TMPU undergoes simultaneous cross-linking and interaction with the perovskite intermediate, forming a dynamically evolving intergranular network. This network blocks moisture intrusion and reduces the energy barrier for α-FAPbI3 formation, preventing premature degradation and eliminating directional inhomogeneity.
How does the phase-locking strategy compare to other scalable fabrication methods in terms of module efficiency and stability under industrial-relevant conditions?
The TMPU-based strategy achieves 21.5% module efficiency, surpassing the 20% threshold for scalable modules. It retains over 90% of initial efficiency after 1500 h of 85°C MPPT (ISOS-L-2) and 2300 h of 85°C/85% RH damp-heat (ISOS-D-3), outperforming many reported large-area modules.
What are the underlying degradation mechanisms in nonuniform perovskite films, and how does morphological homogeneity mitigate them?
Nonuniform films suffer from autocatalytic degradation: early-coated regions with higher defect density and PbI2 accumulation serve as catalytic centers that propagate decomposition to adjacent areas. Phase-locked films with uniform morphology suppress these pathways, maintaining over 84% of initial photoluminescence intensity across all regions under identical aging conditions.
What are the practical implications of the phase-locking strategy for industrial-scale manufacturing in terms of cost and throughput?
The strategy is compatible with high-throughput blade-coating processes, which are cost-effective and scalable. By enabling ambient fabrication without the need for inert atmospheres or vacuum-based methods, it reduces capital and operational costs, facilitating commercial deployment.
How does the stability of TMPU-based modules under damp-heat and thermal cycling compare to industry standards, and what is the expected operational lifetime?
Modules retained over 90% of initial efficiency after 2300 h of 85°C/85% RH damp-heat testing and after 1500 h of 85°C MPPT, indicating excellent durability. These results suggest a projected operational lifetime that meets or exceeds typical requirements for commercial photovoltaic modules, though further long-term field testing is needed.
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