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<p>In the fabrication of FAPbI<sub>3</sub>-based perovskite solar cells, Lewis bases play a crucial role in facilitating the formation of the desired photovoltaic α-phase. However, an inherent contradiction exists in their role: they must strongly bind to stabilize the intermediate δ-phase, yet weakly bind for rapid removal to enable phase transition and grain growth. To resolve this conflict, we introduced an on-demand Lewis base molecule formation strategy. This approach utilized Lewis-acid-containing organic salts as synthesis additives, which deprotonated to generate Lewis bases precisely when needed and could be reprotonated back to salts for rapid removal once their role is fulfilled. This method promoted the optimal crystallization of α-phase FAPbI<sub>3</sub> perovskite films, ensuring the uniform vertical distribution of A-site cations, larger grain sizes and fewer voids at buried interfaces. Perovskite solar cells incorporating semicarbazide hydrochloride achieved an efficiency of 26.1%, with a National Renewable Energy Laboratory-certified quasi-steady-state efficiency of 25.33%. These cells retained 96% of their initial efficiency after 1,000 h of operation at 85 °C under maximum power point tracking. Additionally, mini-modules with an aperture area of 11.52 cm<sup>2</sup> reached an efficiency of 21.47%. This strategy is broadly applicable to all Lewis-acid-containing organic salts with low acid dissociation constants and offers a universal approach to enhance the performance of perovskite solar cells and modules.</p>

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On-demand formation of Lewis bases for efficient and stable perovskite solar cells

  • 期刊论文

  • 发表日期：

    2025年4月17日

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  • Sheng Fu,
  • Nannan Sun,
  • Hao Chen,
  • Cheng Liu,
  • Xiaoming Wang,
  • You Li,
  • Abasi Abudulimu,
  • Yuanze Xu,
  • Shipathi Ramakrishnan,
  • Chongwen Li,
  • Yi Yang,
  • Haoyue Wan,
  • Zixu Huang,
  • Yeming Xian,
  • Yifan Yin,
  • Tingting Zhu,
  • Haoran Chen,
  • Amirhossein Rahimi,
  • Muhammad Mohsin Saeed,
  • Yugang Zhang,
  • Qiuming Yu,
  • David S. Ginger,
  • Randy J. Ellingson,
  • Bin Chen,
  • Zhaoning Song,
  • Mercouri G. Kanatzidis,
  • Edward H. Sargent,
  • Yanfa Yan

摘要

In the fabrication of FAPbI3-based perovskite solar cells, Lewis bases play a crucial role in facilitating the formation of the desired photovoltaic α-phase. However, an inherent contradiction exists in their role: they must strongly bind to stabilize the intermediate δ-phase, yet weakly bind for rapid removal to enable phase transition and grain growth. To resolve this conflict, we introduced an on-demand Lewis base molecule formation strategy. This approach utilized Lewis-acid-containing organic salts as synthesis additives, which deprotonated to generate Lewis bases precisely when needed and could be reprotonated back to salts for rapid removal once their role is fulfilled. This method promoted the optimal crystallization of α-phase FAPbI3 perovskite films, ensuring the uniform vertical distribution of A-site cations, larger grain sizes and fewer voids at buried interfaces. Perovskite solar cells incorporating semicarbazide hydrochloride achieved an efficiency of 26.1%, with a National Renewable Energy Laboratory-certified quasi-steady-state efficiency of 25.33%. These cells retained 96% of their initial efficiency after 1,000 h of operation at 85 °C under maximum power point tracking. Additionally, mini-modules with an aperture area of 11.52 cm2 reached an efficiency of 21.47%. This strategy is broadly applicable to all Lewis-acid-containing organic salts with low acid dissociation constants and offers a universal approach to enhance the performance of perovskite solar cells and modules.