<p>Constructing 2D/3D perovskite heterojunction is an effective method to improve performance and stability of perovskite solar cells (PSCs), while the quantum well in 2D perovskites hinders carrier transport. To address this issue, <i>π</i>-conjugated semiconducting ligands have been introduced to enhance carrier-transfer capability of 2D perovskites. Here, two triphenylamine (TPA)-based ligands are specifically designed through <i>π</i>-extension with a fused (N-TPEAI) or covalently linked (P-TPEAI) benzene ring. For the first time, TPA semiconductor-based ligands have been incorporated to construct 2D/3D PSCs with poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine] (PTAA) as hole-transport materials (HTMs). Combined experimental and computational analyses reveal that this <i>π</i>-conjugation extension strategy proves to be effective in strengthening intermolecular interactions both between the adjacent spacer cations within 2D perovskites and at perovskite/PTAA interfaces, particularly in the case of P-TPEAI. Ultimately, the resultant 2D/3D PSCs employing P-TPEAI achieve an outstanding efficiency of 26.13%, which, to the best of our knowledge, is the highest value reported for 2D/3D PSCs incorporating PTAA HTMs. Moreover, benefiting from the robustness of both 2D perovskites and PTAA, the corresponding devices also exhibit excellent light-heat stability, meeting ISOS-L-2 protocol. These findings provide important guidelines for future design of organic spacers in advancing efficient and robust PSCs and related optoelectronic devices.</p><p><MediaObject ID="MO101"> <ImageObject Color="Color" FileRef="MediaObjects/40820_2026_2145_Figa_HTML.png" Format="PNG" Height="595" Rendition="HTML" Resolution="300" Type="LinedrawHalftone" Width="1298" /> </MediaObject></p>

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Interfacial Coupling Design Enhancing Hole Transport in PTAA-Based Perovskite Solar Cells with Efficiency over 26%

  • Huaiman Cao,
  • Xufan Zheng,
  • Yue Qiang,
  • Liangyu Zhao,
  • Yulong Chen,
  • Zhiguang Sun,
  • Yingguo Yang,
  • Hin-Lap Yip,
  • Ze Yu

摘要

Constructing 2D/3D perovskite heterojunction is an effective method to improve performance and stability of perovskite solar cells (PSCs), while the quantum well in 2D perovskites hinders carrier transport. To address this issue, π-conjugated semiconducting ligands have been introduced to enhance carrier-transfer capability of 2D perovskites. Here, two triphenylamine (TPA)-based ligands are specifically designed through π-extension with a fused (N-TPEAI) or covalently linked (P-TPEAI) benzene ring. For the first time, TPA semiconductor-based ligands have been incorporated to construct 2D/3D PSCs with poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine] (PTAA) as hole-transport materials (HTMs). Combined experimental and computational analyses reveal that this π-conjugation extension strategy proves to be effective in strengthening intermolecular interactions both between the adjacent spacer cations within 2D perovskites and at perovskite/PTAA interfaces, particularly in the case of P-TPEAI. Ultimately, the resultant 2D/3D PSCs employing P-TPEAI achieve an outstanding efficiency of 26.13%, which, to the best of our knowledge, is the highest value reported for 2D/3D PSCs incorporating PTAA HTMs. Moreover, benefiting from the robustness of both 2D perovskites and PTAA, the corresponding devices also exhibit excellent light-heat stability, meeting ISOS-L-2 protocol. These findings provide important guidelines for future design of organic spacers in advancing efficient and robust PSCs and related optoelectronic devices.