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<p>Two-dimensional/three-dimensional (2D/3D) perovskite heterojunctions at the contact interfaces have been proven to enhance the stability and power conversion efficiency (PCE) of perovskite solar cells (PSCs). The 2D/3D bilayer is typically formed via a solution post-treatment onto the 3D perovskite, where the 2D layer’s dimensionality depends on the ligand size and its reactivity. Despite their stability, long-chain ligands typically form 2D perovskites with low dimensionality (<i>n</i> = 1, 2) which feature poor charge conductivity and mobility. Here, we propose an in situ fabrication method incorporating long-chain oleylammonium (OlyA<sup>+</sup>) ligands directly into the perovskite ink. This approach forms 2D perovskite with higher dimensionalities (<i>n</i> ≥ 3) with enhanced (001) crystal facet orientation of the 3D film, improved energetic alignment, charge extraction, and structural stability. The fabricated inverted PSCs with 1.55&#xa0;eV bandgap achieved a maximum PCE of 26.22% for small area and 24.6% for 1cm<sup>2</sup> devices, as well as 21.1% for mini-modules (6.8 cm<sup>2</sup>). Additionally, the PSCs with in situ formed 2D/3D perovskite heterojunctions retained 90% and 80% of their initial PCE after 1200&#xa0;h photothermal stability and 1050&#xa0;h outdoor testing, respectively. Our one-step strategy produces uniform and stable 2D/3D perovskite heterojunctions with enhanced passivation capability, overcoming the limitations of conventional sequential methods and offering a promising and effective approach for highly stable and efficient PSCs.</p><p></p>

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One-Step Formation of 2D/3D Perovskite Heterojunction via Ligand Intercalation and Facet Engineering for Efficient Perovskite Solar Cells

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年2月9日

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  • Drajad Satrio Utomo,
  • Yanping Liu,
  • Andi Muhammad Risqi,
  • Mohammed Ghadiyali,
  • Imil Fadli Imran,
  • Rakesh Rosan Pradhan,
  • Shynggys Zhumagali,
  • Sofiia Kosar,
  • Vladyslav Hnapovskyi,
  • Christopher E. Petoukhoff,
  • Hao Tian,
  • Xiaoming Chang,
  • Badri Vishal,
  • Adi Prasetio,
  • Anil Reddy Pininti,
  • Marco Marengo,
  • Ahmed Ali Said,
  • Aleksandra Oranskaia,
  • Jongbeom Kim,
  • Chuanxiao Xiao,
  • Frédéric Laquai,
  • Thomas D. Anthopoulos,
  • Udo Schwingenschlögl,
  • Sang Il Seok,
  • Randi Azmi,
  • Stefaan De Wolf

摘要

Two-dimensional/three-dimensional (2D/3D) perovskite heterojunctions at the contact interfaces have been proven to enhance the stability and power conversion efficiency (PCE) of perovskite solar cells (PSCs). The 2D/3D bilayer is typically formed via a solution post-treatment onto the 3D perovskite, where the 2D layer’s dimensionality depends on the ligand size and its reactivity. Despite their stability, long-chain ligands typically form 2D perovskites with low dimensionality (n = 1, 2) which feature poor charge conductivity and mobility. Here, we propose an in situ fabrication method incorporating long-chain oleylammonium (OlyA+) ligands directly into the perovskite ink. This approach forms 2D perovskite with higher dimensionalities (n ≥ 3) with enhanced (001) crystal facet orientation of the 3D film, improved energetic alignment, charge extraction, and structural stability. The fabricated inverted PSCs with 1.55 eV bandgap achieved a maximum PCE of 26.22% for small area and 24.6% for 1cm2 devices, as well as 21.1% for mini-modules (6.8 cm2). Additionally, the PSCs with in situ formed 2D/3D perovskite heterojunctions retained 90% and 80% of their initial PCE after 1200 h photothermal stability and 1050 h outdoor testing, respectively. Our one-step strategy produces uniform and stable 2D/3D perovskite heterojunctions with enhanced passivation capability, overcoming the limitations of conventional sequential methods and offering a promising and effective approach for highly stable and efficient PSCs.