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The hygroscopic dopants used in Spiro‐OMeTAD hole‐transport materials (HTMs) in n–i–p perovskite solar cells (PSCs) inevitably cause device degradation. Herein, two polymer interface materials based on lead anchoring groups are developed. It is found that 2D polymers 2DP‐BT and 2DP‐Por can form dense films and exhibit excellent hydrophobicity. Importantly, 2DP‐Por can passivate the surface defects through noncovalent interactions, reducing nonradiative recombination loss. After introducing these polymer interface materials between the perovskite layer and the HTM layer, the optimized devices using 2DP‐Por and 2DP‐BT achieve champion power conversion efficiency of 24.12% and 23.29%, respectively, and the stability is significantly improved. These results indicate that developing polymer interface materials containing lead anchoring groups can improve PSC efficiency and stability and elucidate critical molecular design rules for interface materials. [ABSTRACT FROM AUTHOR]

Quasi‐two‐dimensional perovskite solar cells (quasi‐2D PSCs) have drawn significant attention and are rapidly developing owing to the impressive stability of the materials and devices. However, there are no reliable guidelines for designing and selecting suitable organic spacer cations to achieve high power conversion efficiency (PCE) in quasi‐2D PSCs. Herein, the effects of the spacer cations with different substituents, i.e., benzylamine (PMA), 4‐methoxybenzylamine (p‐MeOPMA), and 4‐fluorobenzylamine (p‐FPMA), on the optoelectronic properties and device performance of quasi‐2D perovskites are systematically investigated. It is found that the spacer cations with different substituents mainly affect the crystal growth and film quality of quasi‐2D perovskites. Interestingly, quasi‐2D perovskites based on p‐MeOPMA or p‐FPMA exhibit poor crystallinity and crystal orientation, while quasi‐2D perovskite based on the unsubstituted PMA shows improved crystallinity and crystal orientation, which enables suppressed trap densities and efficient charge transport. The PMA‐based quasi‐2D perovskite (nominal n = 3) solar cell exhibits the highest PCE of 13.58%. These results demonstrate that the rational regulation of organic spacer cations plays a crucial role in improving the crystallinity and crystal orientation of perovskite films and elucidate key guiding rules for organic spacer cations for high‐performance quasi‐2D PSCs. [ABSTRACT FROM AUTHOR]

[Display omitted] • Wide-bandgap polymers in organic photovoltaics provide a valuable toolbox for developing hole transport materials (HTMs). • Perovskite solar cells (PSCs) using dopant-free PBQx-TCl HTM demonstrated an efficiency of 24.12 % with a high V OC of 1.20 V and good operational stability (T 90 > 600 hours). Dopant-free polymer hole transport materials (HTMs) exhibit high thermal stability, hydrophobicity and film-processing capabilities, demonstrating excellent device efficiency and stability in perovskite solar cells (PSCs). Continued innovation of wide-bandgap polymers in organic photovoltaics (OPV) provides a valuable toolbox for developing polymeric HTMs. Here, we propose an effective molecule design for selecting structurally relevant polymers (D18, D18-Cl, PBQx-TCl) available for commercialization. We discover that the highly planar conjugated backbones play a crucial role in regulating the packing orientation of the film relative to the perovskite. The moderate aggregation with face-on packing orientation is conducive to the high-quality film, which is responsible for better contact with perovskite and superior charge extraction and transport. Simultaneously, these polymers with robust passivation enhanced the open circuit voltage (V OC) without additional passivation layers, streamlining the device process. Consequently, a PSC using dopant-free PBQx-TCl HTL demonstrated an efficiency of 24.12 % with a high V OC of 1.20 V and good operational stability (T 90 > 600 h). This work reveals transparent structure–function-performance relationships between molecules and devices, paving the way for the subsequent development of high-performance HTMs. [ABSTRACT FROM AUTHOR]