Crosslinkable and Chelatable Organic Ligand Enables Interfaces and Grains Collaborative Passivation for Efficient and Stable Perovskite Solar Cells

Abstract The organic–inorganic halide perovskite solar cell (PerSC) is the state‐of‐the‐art emerging photovoltaic technology. However, the environmental water/moisture and temperature‐induced intrinsic degradation and phase transition of perovskite greatly retard the commercialization process. Herein, a dual‐functional organic ligand, 4,7‐bis((4‐vinylbenzyl)oxy)‐1,10‐phenanthroline (namely, C1), with crosslinkable styrene side‐chains and chelatable phenanthroline backbone, synthesized via a cost‐effective Williamson reaction, is introduced for collaborative electrode interface and perovskite grain boundaries (GBs) engineering. C1 can chemically chelate with Sn⁴⁺ in the SnO₂ electron transport layer and Pb²⁺ in the perovskite layer via coordination bonds, suppressing nonradiative recombination caused by traps/defects existing at the interface and GBs. Meanwhile, C1 enables in situ crosslinking via thermal‐initiated polymerization to form a hydrophobic and stable polymer network, freezing perovskite morphology, and resisting moisture degradation. Consequently, through collaborative interface‐grain engineering, the resulting PerSCs demonstrate high power conversion efficiency of 24.31% with excellent water/moisture and thermal stability. The findings provide new insights of collaborative interface‐grain engineering via a crosslinkable and chelatable organic ligand for achieving efficient and stable PerSCs.