Abstract
Abstract The severe degradation and limited optoelectronic performance in water is the Achilles' heel of hybrid organic-inorganic halide perovskite materials, which prevents their further industrial deployment in hostile conditions. In this manuscript, we propose a new molecular dye bearing a dicyano group to improve the water stability and optoelectronic properties of the halide perovskite/TiO2 film. The halide perovskite-based photoelectrochemical setup bearing the dicyano anchor-based dye, 4-(dicyanomethylene)-2-methyl-6-(4-dimethylaminostyryl)-4H-pyran, witnesses a significant enhancement in the photocurrent generated by the halide perovskite CH3NH3PbI3-based film in aqueous solution under the visible light irradiation. Such enhanced optoelectronic performance is accompanied with a much improved stability of the halide perovskite film in water. The first-principles calculations suggest that the molecular dye bearing the dicynao anchor not only adsorbs on the TiO2 substrate, but also strongly interacts with the halide perovskite surfaces; therefore, the bifunctional dicyano anchor could stabilize the CH3NH3PbI3/TiO2 interfacial structure and improve the optoelectronic performance and stability of the halide perovskite electrode. This study benefits the development of the dye-sensitized perovskite materials for the halide-perovskite-based energy devices such as solar cells and water-splitting systems.
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