<p>Low-dimensional perovskites have been widely explored to enhance the performance of perovskite solar cells. However, conventional low-dimensional perovskites rely on amino-based cations with weak hydrogen bonds, which makes them unstable due to facile deprotonation. Here we introduce stable trimethylphosphonium-based cations featuring P-centred ligands with robust –CH<sub>3</sub> groups. These cations exhibit significantly higher acid dissociation constants, suppressed Hofmann elimination and reduced susceptibility to bimolecular nucleophilic substitution, thereby inhibiting degradation while providing strong defect passivation. A single-crystal structural analysis revealed that these cations assemble into a one-dimensional perovskitoid architecture that surrounds and protects the inorganic Pb–I framework, thereby conferring exceptional resistance to moisture, heat and electrical bias. Consequently, single-junction 1.25-eV-bandgap Sn–Pb perovskite solar cells achieved a power conversion efficiency of 24.19%. Moreover, monolithic all-perovskite tandem devices reached a high open-circuit voltage of 2.224 V and a power conversion efficiency of 30.17% (certified 29.18%). These tandem devices retained over 90% of their initial efficiency for more than 2,000 h under continuous maximum power point tracking. Furthermore, the one-dimensional trimethylphosphonium cation-surrounded perovskitoids were used in high-performance 1.77-eV-bandgap perovskite solar cells and green perovskite light-emitting diodes, thus showing that they offer a versatile platform for efficient and stable perovskite optoelectronic devices.</p>

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Stable low-dimensional perovskitoids for high-performance all-perovskite tandem solar cells

  • Guang Li,
  • Wei Ai,
  • Weiwei Meng,
  • Anamika Mishra,
  • Shiqiang Fu,
  • Guoyi Chen,
  • Fang Yao,
  • Wenbo Li,
  • Shun Zhou,
  • Zhiqiu Yu,
  • Haibing Wang,
  • Jiahao Wang,
  • Shining Zhang,
  • Dexin Pu,
  • Senke Cheng,
  • Yunfei Xiong,
  • Yong Liu,
  • Ying Zhang,
  • Ti Wang,
  • Zhenhua Yu,
  • Weijun Ke

摘要

Low-dimensional perovskites have been widely explored to enhance the performance of perovskite solar cells. However, conventional low-dimensional perovskites rely on amino-based cations with weak hydrogen bonds, which makes them unstable due to facile deprotonation. Here we introduce stable trimethylphosphonium-based cations featuring P-centred ligands with robust –CH3 groups. These cations exhibit significantly higher acid dissociation constants, suppressed Hofmann elimination and reduced susceptibility to bimolecular nucleophilic substitution, thereby inhibiting degradation while providing strong defect passivation. A single-crystal structural analysis revealed that these cations assemble into a one-dimensional perovskitoid architecture that surrounds and protects the inorganic Pb–I framework, thereby conferring exceptional resistance to moisture, heat and electrical bias. Consequently, single-junction 1.25-eV-bandgap Sn–Pb perovskite solar cells achieved a power conversion efficiency of 24.19%. Moreover, monolithic all-perovskite tandem devices reached a high open-circuit voltage of 2.224 V and a power conversion efficiency of 30.17% (certified 29.18%). These tandem devices retained over 90% of their initial efficiency for more than 2,000 h under continuous maximum power point tracking. Furthermore, the one-dimensional trimethylphosphonium cation-surrounded perovskitoids were used in high-performance 1.77-eV-bandgap perovskite solar cells and green perovskite light-emitting diodes, thus showing that they offer a versatile platform for efficient and stable perovskite optoelectronic devices.