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<p>Inorganic perovskite solar cells could benefit from surface passivation using 2D/3D perovskite heterostructures. However, conventional spacer cations fail to exchange with the tightly bonded Cs cation in the inorganic perovskite to form 2D layers atop; or, when they do enable formation of a 2D layer, they migrate under heat, degrading device performance. Here we investigate the mechanisms behind 2D/3D heterostructure formation and stabilization. We find that 2D/3D heterostructure formation is driven by interactions between ammonium groups and [PbI<sub>6</sub>]<sup>4−</sup> octahedra. We thus incorporate electron-withdrawing fluorine to enhance inorganic–organic cation interdiffusion and promote heterostructure formation. We note that stability relies on interactions between the entire spacer cations and [PbI<sub>6</sub>]<sup>4−</sup> octahedra. We therefore introduce anchoring groups that double cation desorption energies, preventing cation migration at elevated temperatures. CsPbI<sub>3</sub>/(perfluoro-1,4-phenylene)dimethanammonium lead iodide heterostructures enable an efficiency of 21.6% and a maximum power point operating stability at 85 °C of 950 h. We demonstrate 16-cm<sup>2</sup> modules with an efficiency of 19.8%.</p>

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Cation interdiffusion control for 2D/3D heterostructure formation and stabilization in inorganic perovskite solar modules

  • 期刊论文

  • 发表日期：

    2025年7月16日

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  • Cheng Liu,
  • Yi Yang,
  • Jared D. Fletcher,
  • Ao Liu,
  • Isaiah W. Gilley,
  • Charles Bruce Musgrave III,
  • Zaiwei Wang,
  • Huihui Zhu,
  • Hao Chen,
  • Robert P. Reynolds,
  • Bin Ding,
  • Yong Ding,
  • Xianfu Zhang,
  • Raminta Skackauskaite,
  • Haoyue Wan,
  • Lewei Zeng,
  • Abdulaziz S. R. Bati,
  • Naoyuki Shibayama,
  • Vytautas Getautis,
  • Bin Chen,
  • Kasparas Rakstys,
  • Paul J. Dyson,
  • Mercouri G. Kanatzidis,
  • Edward H. Sargent,
  • Mohammad K. Nazeeruddin

摘要

Inorganic perovskite solar cells could benefit from surface passivation using 2D/3D perovskite heterostructures. However, conventional spacer cations fail to exchange with the tightly bonded Cs cation in the inorganic perovskite to form 2D layers atop; or, when they do enable formation of a 2D layer, they migrate under heat, degrading device performance. Here we investigate the mechanisms behind 2D/3D heterostructure formation and stabilization. We find that 2D/3D heterostructure formation is driven by interactions between ammonium groups and [PbI6]4− octahedra. We thus incorporate electron-withdrawing fluorine to enhance inorganic–organic cation interdiffusion and promote heterostructure formation. We note that stability relies on interactions between the entire spacer cations and [PbI6]4− octahedra. We therefore introduce anchoring groups that double cation desorption energies, preventing cation migration at elevated temperatures. CsPbI3/(perfluoro-1,4-phenylene)dimethanammonium lead iodide heterostructures enable an efficiency of 21.6% and a maximum power point operating stability at 85 °C of 950 h. We demonstrate 16-cm2 modules with an efficiency of 19.8%.