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Improved Conductivity of 2D Perovskite Capping Layer for Realizing High-Performance 3D/2D Heterostructured Hole Transport Layer-Free Perovskite Photovoltaics

Xi ChenKey Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education, LIFM, School of Chemistry, IGCMEWenhuai FengKey Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education, LIFM, School of Chemistry, IGCMEYuxuan FangKey Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education, LIFM, School of Chemistry, IGCMEQing LiEast China University of Science and TechnologyYuhua HuangKey Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education, LIFM, School of Chemistry, IGCMEXueqing ChangKey Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education, LIFM, School of Chemistry, IGCMEChan‐Ying YaoKey Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education, LIFM, School of Chemistry, IGCMEYujian ShenKey Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education, LIFM, School of Chemistry, IGCMEGengling LiuKey Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education, LIFM, School of Chemistry, IGCMEShuang YangEast China University of Science and TechnologyXu‐Dong WangKey Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education, LIFM, School of Chemistry, IGCMEMingjian YuanKey Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), College of ChemistryWu‐Qiang WuKey Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education, LIFM, School of Chemistry, IGCME
2025en
ABI

Аннотация

Perovskite solar cells (PSCs) have emerged as low-cost photovoltaic representatives. Constructing three-dimensional (3D)/two-dimensional (2D) perovskite heterostructures has been shown to effectively enhance the efficiency and stability of PSCs. However, further enhancement of device performance is still largely limited by inferior conductivity of the 2D perovskite capping layer and its mismatched energy level with the 3D perovskite layer. Here, we developed an effective surface modification strategy via synergically incorporating inorganic high valence-state niobium ion (Nb5+) metal dopants and organic ammonium halide salts to in situ construct a high-quality 2D perovskite capping layer on top of the underlying 3D perovskite layer. As a result, the conductivity of the 2D perovskite capping layer was effectively enhanced by 43%, the energy barrier between 3D and 2D perovskite layers was favorably reduced, and the built-in electric field of the 3D/2D heterostructured perovskite stacks has been enlarged. In addition, the 2D perovskite capping layer also effectively reduced the defect densities by up to 29%, as verified by the space-charge-limited-current (SCLC) tests. Benefiting from the facilitated charge extraction and suppressed non-radiative recombination, the blade-coated hole transport layer-free PSCs based on this optimized 3D/2D heterostructured perovskite film achieved an efficiency of 23.2%, ∼19% higher than that of the control device (19.5%), which represented one of the best-performing PSCs with simplified device architecture fabricated via a scalable fabrication technique. The modified 3D/2D perovskite-based device also exhibited improved operational stability.

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