Key Takeaways & Executive Findings
- •• A natural and regenerable redox shuttle using glutathione (GSH) effectively eliminates harmful Sn4+ and Sn0/Pb0 impurities in Pb-Sn perovskite solar cells. • GSH incorporation regulates perovskite crystallization, leading to high-quality charge separation junctions and improved device performance. • GSH-modified Pb-Sn solar cells achieve a champion PCE of 23.71%, and all-perovskite tandem cells reach 28.49% with 90% retention after 560 hours. • This nature-inspired redox shuttling strategy provides a new pathway for developing efficient and stable all-perovskite tandem solar cells.
Abstract
Pb–Sn mixed perovskite solar cells (PSCs) are crucial components for realizing efficient all-perovskite tandem devices. However, their efficiency and stability are severely limited by oxidative degradation (Sn4+ formation) and metallic defects (Sn0/Pb0). In addition, the rapid and uncontrolled Sn2+ nucleation kinetics result in nonuniform crystallization. Herein, we introduce a natural redox shuttle glutathione (GSH) in Pb–Sn mixed PSCs, achieving regenerable antioxidation and crystallization regulation simultaneously. The reversible redox reactions between GSH and glutathione disulfide (GSSG) enable the self-healing of Sn4+ and Sn0/Pb0 impurities, creating a regenerable antioxidation protective shell at the perovskite interfaces. Meanwhile, the strong coordination between GSH and perovskite regulates the crystallization process, optimizing the nucleation and crystallization kinetics. Furthermore, the GSH incorporation creates a high-quality charge separation junction at the perovskite/hole transport layer, facilitating carrier separation and extraction. The optimized Pb–Sn PSCs exhibit impressive power conversion efficiencies (PCEs) of up to 23.71%. The champion all-perovskite tandem PSCs with GSH achieve a PCE of 28.49% and retain 90% of the initial PCE after 560 h of continuous illumination. This work establishes a new nature-inspired redox shuttling strategy and elucidates its working mechanism, advancing the development of efficient and stable all-perovskite tandem solar cells.
1. Introduction
All-perovskite tandem solar cells (TSCs) have emerged as promising candidates to break the Shockley–Queisser (SQ) efficiency limit of single-junction solar cells, while maintaining the intrinsic advantages of perovskite materials, such as low cost, compatibility with flexible substrates and solution processability [1, 2]. Recently, their power conversion efficiencies (PCEs) have reached 30.1% [3], demonstrating substantial commercial potential [4]. However, compared with other TSC technologies, the development of all-perovskite TSCs is still primarily impeded by the performance limitations of Pb–Sn mixed perovskite solar cells (PSCs) [5, 6].
These challenges mainly stem from the easy oxidation of Sn2+ to Sn4+, resulting in numerous Sn vacancies [7]. Meanwhile, the disproportionation reaction of Sn2+ and perovskite degradation introduce unfavorable impurities of Sn4+, Sn0, and Pb0, compromising the optoelectronic properties and device stability [8]. In addition, compared with pure Pb-based perovskite, Sn2+ ions exhibit weaker coordination with common solvents such as dimethyl sulfoxide (DMSO) and dimethylformamide (DMF), making them more easily released from the solvent complex, which leads to rapid nucleation and growth of Sn-rich domains. This rapid crystallization process restricts the time available for ion diffusion and lattice reordering, ultimately resulting in the formation of structural defects, such as vacancies, grain boundaries, and pinholes [9]. These defects lead to severe non-radiative recombination, thereby hindering the carrier transport and limiting the photovoltaic performance.
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Rui Meng, Liming Du, Can Li, Zhi Wan, Jishan Shi, Yueying Zhang, Wenfeng Liu, Chongyang Zhi, Chunmei Jia, Lili Tan, Chuanxiao Xiao, Xian-Zong Wang, Lin Song, Xingyu Gao, Zhen Li (2026). Nature-Inspired Redox Shuttle with Regenerable Antioxidant for Efficient All-Perovskite Tandem Solar Cells. Nano-Micro Letters. https://doi.org/10.1007/s40820-025-02006-6
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Frequently Asked Questions
What is the main challenge in Pb-Sn mixed perovskite solar cells?
The main challenges are the easy oxidation of Sn2+ to Sn4+, formation of metallic defects (Sn0/Pb0), and rapid uncontrolled crystallization, which lead to non-radiative recombination and reduced device performance.
How does glutathione (GSH) improve the performance of Pb-Sn perovskite solar cells?
GSH acts as a regenerable redox shuttle, converting harmful Sn4+ and Sn0/Pb0 impurities back to Sn2+ via reversible redox reactions. It also regulates crystallization through strong coordination with perovskite, resulting in high-quality films and improved charge separation.
What power conversion efficiencies were achieved with GSH modification?
The GSH-modified Pb-Sn perovskite solar cells achieved a champion PCE of 23.71%, and all-perovskite tandem solar cells reached a PCE of 28.49% with 90% retention after 560 hours of continuous operation.
What is the significance of the nature-inspired redox shuttle strategy?
This strategy provides a new approach to simultaneously address oxidation and crystallization issues in Pb-Sn perovskites, advancing the development of efficient and stable all-perovskite tandem solar cells.
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