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Inorganic CuSCN and organic tetrathiafulvalene derivatives (TTFs) have been exploited as hole-transport materials (HTM) in hybrid perovskite solar cells. To develop new HTM, we herein report two hybrid materials incorporating redox-active TTFs with CuSCN framework (TTFs-CuSCN). Single-crystal analysis showed that compound [Cu2(py-TTF-py)(SCN)2] (1) is three-dimensional (3D) and compound [Cu(py-TTF-py)(SCN)] (2) is two-dimensional (2D) (py-TTF-py = 2,6-bis(4?-pyridyl)tetrathiafulvalene). There are covalent coordination interactions between CuSCN and py-TTF-py and short S···S contacts between the py-TTF-py ligands for both compounds. Besides, C···S contacts exist between py-TTF-py ligands of the neighboring 2D networks in 2, which facilitate the charge transfer and supply efficient multidimensional pathways for carrier migration. As a result, 2 presented better semiconductor performance in comparison with that of 1. The performance of 2 related to the HTMs could be significantly improved by modulating the electronic state of the TTFs-CuSCN framework via oxidative doping. The iodine-doped 2D material (2-I2) gives the most excellent conductivity and carrier mobility, which might be a potential new HTM.
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Reference：
Copper catalysis in organic synthesis – NCBI,
Special Issue “Fundamentals and Applications of Copper-Based Catalysts”