Adhesively Bridging Co-Self-Assembled Monolayer and Perovskite Via In Situ Polymerization for Enhanced Stability of Inverted Perovskite Solar Cells.

Xu, Xiaowei; Li, Sibo; Shan, Chengwei; Peng, Wenbo; Chen, You; Li, Shangzhi; Peng, Haichen; Dai, Tingting et al. · Adv Mater · 2025

basic_science · Level V

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Abstract

The strategic utilization of self-assembled monolayers (SAMs) significantly advances the interfacial contact and power conversion efficiency (PCE) of inverted perovskite solar cells (IPSCs). However, inadequate adhesion between the SAM and perovskite layer remains a critical challenge, limiting further performance enhancement. Herein, a synergistic interface engineering strategy is introduced that combines a co-assembly approach with in situ polymerization to optimize the buried interface of perovskite film. Specifically, 11-Mercaptoundecylphosphoric acid (MPA) is incorporated into a SAM to form co-SAMs, improving homogeneity and mitigating defects at the NiO<sub>x</sub> surface. Simultaneously, the ionic liquid (IL) monomer 1-Allyl-3-vinylimidazolium bis((trifluoromethyl)sulfonyl) imide (AVMTF<sub>2</sub>) is incorporated into the perovskite precursor. The aggregation of ILs cation at the bottom interface facilitates in situ polymerization via sulfhydryl end groups, forming the POL-AVM polymer at the perovskite/SAM interface. This polymer enhances interfacial adhesion, regulates perovskite crystallization, and reinforces structural integrity by strongly anchoring organic cations through multiple hydrogen bonds. As a result, this synergistic strategy achieves a champion PCE of 26.25% (certified 26.04%), along with excellent long-term stability, retaining 95.6% of its initial efficiency after 1000 h of continuous operation under the ISOS-L-2I protocol.